Nolan played a key role in Newcastle's push for promotion the following season; he scored his first league goal for Newcastle on 22 August against Crystal Palace, and the first hat-trick of his career, as part of a 4–0 away win against Ipswich Town on 26 September. Nolan captained Newcastle for the first time in a 5–1 win against Cardiff City taking over for the absent Nicky Butt and Alan Smith. After an 11-game goal drought, Nolan picked up his 11th league goal of the season on 20 February against Preston North End in a 3–0 win. He followed this up with the final goal in Newcastle's 6–1 home drubbing of Barnsley two games later. He was voted as the Championship Player of the Year at the Football League Awards on 16 March. On 5 April 2010, Newcastle United secured automatic promotion to the Premier League, after fellow contenders Nottingham Forest failed to beat Cardiff City. Newcastle took to the field hours later, in front of 48,750 fans, and Nolan scored the winner with a scissor-kick in the 2–1 win over Sheffield United.
Nolan was named as the new Newcastle United club captain for the 2010–11 season, succeeding the retired Nicky Butt. Nolan scored his first goals of the season as he netted a brace in Newcastle's 6–0 win against Aston Villa in their first home game. On 31 October 2010, Nolan scored his first Premier League hat-trick, achieving the feat in the Tyne–Wear derby against Sunderland in a 5–1 home win. Nolan scored the opener against Liverpool in new manager Alan Pardew's first game in charge on 11 December 2010, which Newcastle went on to win 3–1. Nolan scored the opening goal in the second derby of the season against Sunderland on 16 January, which finished 1–1. On 26 February 2011, Nolan scored his 50th Premier League goal, against his former club, Bolton Wanderers at St James' Park, which finished 1–1.