At the 2010 general election, Lloyd's campaign centred on local issues and highlighting of the expenses claims of his Conservative Party opponent, Nigel Waterson. He also asked to be lent votes by local supporters of the Labour and Green parties. Liberal Democrat leader Nick Clegg hosted his eve of poll rally, where former Conservative MP Ernle Money, who had moved to Eastbourne, pledged his support to Lloyd. On 7 May, Lloyd was elected the MP for Eastbourne with a majority of 3,435 votes.
From 2010 to 2015, Lloyd served as the Liberal Democrats' spokesperson for Northern Ireland in the House of Commons. Over the same period, Lloyd served on the Work and Pensions Select Committee in the House of Commons. He was thought by the Labour opposition to be wavering about supporting changes to housing benefit presented to the committee, but declared that he supported the "direction of travel" of the government. He campaigned for concessions from the Department for Work and Pensions in relation to Personal Independence Payment descriptors to ensure that people with reduced mobility would still be entitled to their Motability vehicles.
In 2010, Lloyd lobbied the Government to reconsider its planned reforms to student visa regulations, which threatened the future of English language schools, arguing it was "nonsensical" to require overseas students to speak the language before they came to study it.
Lloyd founded the All Party Parliamentary Group on religious education in schools in 2010. He has led campaigns to improve, encourage and support RE teaching of the world's major faiths, and of the non-religious, in schools in England and Wales. The chair of the Religious Education Council praised him in The Times as a "key player" in promoting the importance of effective RE teaching in schools.
In 2010, Lloyd created an "MP's Commission", composed of local business and community leaders in his Eastbourne constituency. Its initiatives included: bringing back the Eastbourne 'Sunshine' Carnival; and organising a procurement conference to encourage further economic cooperation between the private sector and major public sector bodies in the town. In 2011, Lloyd developed a successful local apprenticeship initiative, aiming to recruit 100 apprenticeships in 100 days in Eastbourne. The initiative ultimately created 181 apprenticeships and received praise from then-Prime Minister David Cameron. In 2014, Lloyd was awarded the Grassroot Diplomat Initiative Honouree for this work. During the same year, Lloyd was also associated with lobbying for additional funds for local housing projects and supporting negotiations over the regeneration of Eastbourne’s Arndale shopping centre.