On January 15, 2014, Duff signed on to co-star opposite Sutton Foster in the comedy-drama pilot Younger. The series is based on a Pamela Redmond Satran novel, and created and executive-produced by Darren Star for TV Land. Duff was cast as Kelsey Peters, an "ambitious 20-something" who persuades Foster's character to work in a publishing firm. In April 2014, it was announced that the pilot was picked up for a series with a 12-episode deal and would premiere in the fall; the premiere date was later changed to 2015. The show marks Duff's first starring role in a television series since her appearance on Lizzie McGuire. Younger premiered on March 31, 2015. The series has received generally positive reviews from critics and her performance as Kelsey Peters has earned her acclaim, and nominations for Favorite Cable TV Actress at the 2016 and 2017 People's Choice Awards, two Teen Choice Awards nominations, and a nomination for the Gracie Allen Awards.
Duff attended the 2014 iHeartRadio Music Awards on May 1, 2014, where she confirmed that she was working with songwriter Savan Kotecha and English singer Ed Sheeran. On July 23, 2014, it was revealed that Duff had signed with RCA Records to release her upcoming fifth studio album. She released the album's lead single "Chasing the Sun" and its accompanying music video on July 29, 2014. The song entered the Billboard Hot 100 at number 79, becoming her first song to enter the chart since "Stranger" (2007). The song's music video garnered fourteen million views in its first week of release on popular video sharing website YouTube, making it her fastest viewed music video to date. The album's second single, "All About You," was released as the album's official lead single on August 12. It failed to enter the Hot 100 chart, but became her first song to chart on the Mainstream Top 40 chart since "With Love" (2007). It became a top-twenty hit in Australia, where it later earned a Gold certification from the ARIA. This made it her second song to receive a certification in the country, following "So Yesterday" (2003) eleven years prior. In November 2014, Duff provided voice work for a Dora the Explorer special episode as Ice Witch.
Duff's 2014 releases, featured a more folk influenced, "earthy" indie pop sound compared to her last release. The album's lead single was planned to be "All About You" (2014) and, among other instruments, it featured a banjo and an acoustic sound. Instead of the original plans, Duff released a dance-pop record which balanced EDM with the folk pop sound originally planned for the record. This album consolidated Duff as a dance-pop singer.
Following the birth of her son, Duff said that it took her a year for her to lose her baby weight and that she lost nearly 50 pounds by 2013. Duff stated that she revamped her diet and hired a personal trainer to train her in boxing, which was one of the ways she lost her weight in addition to piloxing and spin cycling. Duff's slow but healthy method in shedding off her post-pregnancy weight was praised by health experts and was looked up by actress Tia Mowry, who cited Duff as her idol in taking up a healthy and safer way to lose the excess weight gained during pregnancy. Duff is very vocal about her disapproval of paparazzi photographing children. In 2014, Duff expressed her anger on Twitter regarding two paparazzi who were taking pictures of her son without her consent. She tweeted, "I chose to let them off with a stern warning, next time I will not be so nice. #NoKidsPolicy" The hashtag refers to a bill that was pushed by fellow actresses Halle Berry and Jennifer Garner, which prohibits paparazzi from taking pictures of celebrities' children. In February 2020, Duff uploaded an Instagram video post, documenting her confrontation with a paparazzi who was taking photographs of her children at her son's football game. She clarified the situation in a series of Instagram stories uploads the day after, saying that it was "really highly frustrating" and that the police dismissed her by reasoning that she was at a public park when the incident happened. She voiced out her dissatisfaction and demanded for the law to be changed. The video has since been viewed for more than 2 million times as of November 2020.