On May 30, 1934, Long took to the Senate floor to debate the abrogation of the Platt amendment. But instead of debating the amendment, Long declared his stance on the Chaco War. He proclaimed support for Paraguay against Bolivia, as he maintained that US President Rutherford B. Hayes had awarded the Chaco region to Paraguay in 1878. Long blamed the entire war on "the forces of imperialistic finance", claiming that Paraguay was the rightful owner of the Chaco. He said that Standard Oil, whom Long called "promoter of revolutions in Central America, South America and Mexico," had "bought" the Bolivian government and started the war because Paraguay was unwilling to grant them oil concessions. Long ended his speech by claiming the entire Chaco War was due to the machinations of Wall Street, called the American arms embargo to both sides as subservience to the "big papa" of Wall Street and stated: "Well should we begin on Memorial Day, the hour of mourning, to understand that the imperialistic principles of the Standard Oil Company have become mightier than the solemn treaties and pronouncements of the United States government".
In a second speech given on June 7, 1934, in response to the Bolivian protests, Long again supported Paraguay and attacked Standard Oil as "foreign murderers" and "imperialist oppressors of the freedom of the South American people". Besides abusing Standard Oil, Long announced that since Bolivia was taking the Chaco dispute to the World Court, he was opposed to the United States joining the World Court, saying:
After capturing a Bolivian fort in July 1934, the Paraguayans renamed it Fort Long. Thanks to Long's outspoken stance on the war, he had established himself as one of the most ardent isolationists in the Senate. He further argued that the United States involvement in the Spanish–American War and the First World War had been deadly mistakes conducted on behalf of Wall Street. Consequently, Long demanded the immediate independence of the Philippines, which had been occupied by the United States since 1899. He also opposed American entry into the World Court.
In February 1934, Long introduced his Share Our Wealth plan over a nationwide radio broadcast. He proposed capping personal fortunes at $50 million and repeated his call to limit annual income to $1 million and inheritances to $5 million. (He also suggested reducing the cap on personal fortunes to $10 million–$15 million per individual, if necessary, and later lowered the cap to $5 million–$8 million in printed materials.) The resulting funds would be used to guarantee every family a basic household grant, or "household estate" as Long called it, of $5,000 and a minimum annual income of $2,000–3,000, or one-third of the average family homestead value and income. Long supplemented his plan with proposals for free college education, with admission based on an IQ test, and vocational training for all able students, old-age pensions, veterans' benefits, federal assistance to farmers, public works projects, greater federal regulation of economic activity, a month's vacation for every worker, and limiting the work week to thirty hours to boost employment. He proposed a $10 billion land reclamation project to end the Dust Bowl. Long promised free medical service and what he called a "war on disease" led by the Mayo brothers. In his speech, Long used populist language depicting the U.S. past as a lost paradise stolen by the rich, saying:
Long's plans for the "Share Our Wealth" program attracted much criticism from economists at the time, who stated that Long's plans for redistributing wealth would not result in every American family receiving a grant of $5,000 per year, but rather $400/per year, and that his plans for confiscatory taxation would cap the average annual income at about $3,000. They noted that the confiscated fortunes would only yield $1.50 per each poor family. In 1934, Long held a public debate with Norman Thomas, the leader of the Socialist Party of America, on the merits of Share Our Wealth versus socialism.
With the Senate unwilling to support his proposals, in February 1934 Long formed a national political organization, the Share Our Wealth Society. A network of local clubs led by national organizer Reverend Gerald L. K. Smith, the Share Our Wealth Society was intended to operate outside of and in opposition to the Democratic Party and the Roosevelt administration. By 1935, the society had over 7.5 million members in 27,000 clubs across the country. Long's Senate office received an average of 60,000 letters a week, resulting in Long hiring 48 stenographers to type responses. Of the two trucks that delivered mail to the Senate, one was devoted solely to mail for Long. Long's newspaper, now renamed American Progress, averaged a circulation of 300,000, with some issues reaching over 1.5 million. Long's radical programs were very attractive to union-members; Teamsters president Daniel J. Tobin expressed his growing concerns to Roosevelt. Long drew international attention: writer H. G. Wells traveled across the Atlantic just to interview Long. Wells noted that Long was "like a Winston Churchill who has never been at Harrow. He abounds in promises."
In 1934, Long and James A. Noe, an independent oilman and member of the Louisiana Senate from Ouachita Parish, formed the controversial Win or Lose Oil Company. The firm was established to obtain leases on state-owned lands so that its directors might collect bonuses and sublease the mineral rights to the major oil companies. Although ruled legal, these activities were done in secret, and the stockholders were unknown to the public. Long made a profit on the bonuses and the resale of those state leases and used the funds primarily for political purposes.