During the 2006–07 season, Langenbrunner scored a career-best 60 points, where he also played in all 82 games that season, scoring 23 goals and adding 37 assists (both career bests). In the 2007 playoffs, Langenbrunner again played well, scoring eight points in 11 games before losing to the Stanley Cup Finals-bound Ottawa Senators.
On December 5, 2007, Langenbrunner was named captain of the New Jersey Devils. That year, however, Langenbrunner missed nearly 20 games to a groin injury and his stats dipped as he scored 41 points in 64 games. In the playoffs, the Devils lost in the first round to the New York Rangers 4–1, though Langenbrunner played well, scoring four points in the short series.