In 2016, Jones was acquired by the Connecticut Sun after having her draft rights traded by the Los Angeles Sparks in exchange for Chelsea Gray and two draft picks. In her rookie season, Jones was the backup center for the Sun. She averaged 6.8 ppg, 3.7 rpg and 1.1 bpg in 34 games with 6 starts. In her second season, Jones became the starting center for the Sun. Jones had a breakout season in 2017 in her new starting role. After an 0–4 start, Jones led the Sun to their first win of the season, scoring 23 points along with 21 rebounds in a 97–79 win over the Chicago Sky, making her the 13th player in league history to record a 20-point, 20-rebound performance. On July 8, 2017, the Sun made history as they completed the biggest comeback in franchise history after defeating the Washington Mystics 96–92 after overcoming a 22-point deficit as they improved to 10–7, Jones scored a team-high 22 points along with 9 rebounds in the win. Jones was selected to the 2017 WNBA All-Star Game, her first career All-Star Game appearance. She finished the season averaging a double-double in points and rebounds and also averaged career-highs in scoring, rebounding and blocked shots, quickly emerging as one of the rising young stars in the league. She broke the single season record for rebounds, grabbing 403 rebounds in the 2017 season, breaking Tina Charles previous record of 398. Jones would also win the 2017 WNBA Most Improved Player Award. Her breakout season performance, along with Jasmine Thomas and Alyssa Thomas both emerging as all-stars would lead the Sun back to the playoffs for the first time since 2012. They finished with a 21–13 record as the fourth seed in the league, receiving a bye to the second round elimination game. In her first career playoff game, Jones scored 19 points and grabbed 15 rebounds in an 88–83 loss to the number 5-seeded Phoenix Mercury. In 2018, Jones would have a reduced role on the team despite her success from last season. She started in 16 of the 34 games played but would still effective for the Sun both in the starting lineup and off the bench. By the end of the season, Jones won the WNBA Sixth Woman of the Year award. The Sun made it back to the playoffs as the number 4 seed with a 21-13 record, receiving a bye to the second round. However the Sun would lose yet again to the Phoenix Mercury in the second round elimination game by a final score of 96-86. In 2019, Jones would redeem her starting Center role for the whole season. She would lead the league in rebounds once again and averaged a career-high in blocks, steals and minutes by the end of the season. Jones was also voted into the 2019 WNBA All-Star Game, making it her second all-star appearance and would also make WNBA Second Team. The Sun were a championship contender in the league, finishing with a 23-11 record and the number 2 seed, receiving a double bye to the semi-finals. In the semi-finals, the Sun swept the Los Angeles Sparks 3-0 to advance to the WNBA Finals, making it the franchise's first finals appearance since 2005. The WNBA Finals series was a hard-fought battle, but the Sun fell to the Washington Mystics in five games. In June of 2020, Jones announced that she would forgo the WNBA season due to concerns from the coronavirus.