The three-time champion became just the fifth man to achieve that feat and moved above John McEnroes total of 59 wins.
Unsurprisingly, Roger Federer sits at the top of the list.
The eight-time champion has racked up an impressive 93 wins during his two-decade association with his favourite Grand Slam.
Jimmy Connors (84), Boris Becker (71) and Pete Sampras (63) are the only other players who sit above the Serb.
Most Wimbledon match wins (win/loss)
Incredibly, considering Sampras has seven titles to his name, Djokovic can overtake him on the list with a run to the semi-finals this time around, although the American great has only lost seven matches to the Serbs 10.
Djokovics work on court itself was rather straightforward, as he beat Zeballos 6-1 6-2 6-3, though there was a slight concern as he called the trainer on court to massage his left thigh.
It was somewhat surprising to see the 12-time champion scheduled to play on Court 2 against the Argentine – though he got on with his business effectively.
Zeballos isnt an opponent who would have struck much fear into the heart of the 12-time Grand Slam champion, particularly after their last encounter.
After losing 6-3 6-4 to the Serb in Doha, Zeballos made the curious move to ask his opponent for an on-court selfie.
Djokovic made a point of reminding him of that moment not long before they went on court and Zeballos quickly found himself 6-1 down after 22 minutes.
A swift break followed at the start of the second, with Djokovic in cruise control.
Inevitably, an early break came in the third but there was a slight concern for the former world No. 1 as he required treatment on his left thigh.
However, it didnt seem to affect his progress as he wrapped up the match.
He may well meet British hopeful Kyle Edmund in the last-32, if the 21st seed beats Bradley Klahn.