The Heat’s season win streak stretched to eight games in a row with a 16th consecutive victory in meetings with Charlotte, whose win drought against Miami now spans four years.
James sank eight 3-pointers, hitting 22-of-33 shots from the field overall, and also grabbed seven rebounds and passed off five assists.
“It was a special performance,” Heat coach Erik Spoelstra said. “He was efficient. The rim certainly looked like an ocean to him.”
The former Heat single-game scoring record was 56 points by Glen Rice in April of 1995.
On a night when Miami star guard Dwyane Wade was rested, Chris Bosh contributed 15 points and seven rebounds.
Miami shot 55.4 percent from the floor, including 16-of-28 from 3-point range.
Charlotte’s Al Jefferson scored 38 points and grabbed 19 rebounds.
The Heat improved to 43-14, trailing only Eastern Conference rival Indiana (46-13) for the best record in the NBA and a home-court edge throughout the playoffs.
Charlotte fell to 27-33 as the Bobcats and Atlanta fight for the final two playoff positions in the East.
Miami led 60-54 at half-time before James went wild in the third quarter, going 5-of-5 from beyond the 3-point arc on his way to 25 points in the quarter, matching the Bobcats’ total team output.
James scored Miami’s first eight points of the second half, then added back-to-back three-point plays late in the period for an 89-69 Heat lead.
James followed with his eighth 3-pointer for a 95-73 edge with 1:16 to play in the third and began the fourth quarter with four straight points to reach 53 for the night.
But with Charlotte still fighting to stay in the game, James remained in the lineup and added a pair of layups and a spinning bank shot for a 115-99 Miami edge with 2:23 to play.
After Jefferson hit a jumper for Charlotte, James was fouled and sank two free throws to cap his scoring as fans chanted “M-V-P” to the four-time NBA Most Valuable Player.
James set several other Heat team records, including 22 baskets in a game, most points in a quarter by a player with 25 and most second-half points with 37.
It was his 10th time in his career that James cracked the 50-point barrier.
Since James left the Cleveland Cavaliers for Miami, the Heat have lost the NBA Finals to Dallas, then won the past two league playoff crowns.