On April 1, 2016, DeLeone was promoted to the Kansas City Chiefs assistant linebackers coach. The Chiefs went 12–4 in 2016 and clinched the AFC West title for the first time since 2010 and made the playoffs for the second year in a row for the first time since 1995. They would lose in the Divisional Round against the Pittsburgh Steelers 16–18. During the season they would defeat the NFC Champions, the Atlanta Falcons 29-28. Linebackers Justin Houston, Derrick Johnson, and Tamba Hali would make the NFL's Top 100, ranked 26th, 80th, and 84th respectively. The Chiefs went 10–6 in 2017 and won back-to-back AFC West titles for the first time in franchise history and made the playoffs for the third year in a row for the first time since 1994. They would lose to the Tennessee Titans in the Wild Card round 21-22. They would defeat both the AFC champion New England Patriots and the NFC championPhiladelphia Eagles during the season. Under his coaching, Justin Houston would rank 7th in tackles for loss. Justin Houston would make the NFL's Top 100 ranked 76th. In the 2017 offseason, Derrick Johnson left in free agency & Tamba Hali was released. On January 29, 2018, DeLeone was promoted to the Kansas City Chiefs inside linebackers coach. The Chiefs went 12-4 and won their third straight AFC West title in franchise history and made the playoffs for the fourth year in a row for the first time since 1993. They would go on to defeat the Indianapolis Colts in the Divisional Round 31-13 and then lose to the New England Patriots in the AFC Championship game 31–37. During the season they defeated two playoff teams; the AFC North champion Baltimore Ravens and the Los Angeles Chargers. Under his coaching, Justin Houston ranked 5th in forced fumbles and linebacker Reggie Ragland recorded the 8th longest interception return. At the end of the season, defensive coordinatorBob Sutton was fired and DeLeone left to join his former offensive coordinatorMatt Nagy.
Chicago Bears
On January 29, 2019, the Chicago Bears named DeLeone the inside linebackers coach. The Bears went 8-8 in 2019 and missed the playoffs.