The series' first season focused on Peter Parker's position as photographer for the Daily Bugle, ignoring many other aspects of the characters private life. Spider-man encountered many of his classic villains such as the Vulture and Lizard.
Spider-man also had a run in with Dr. Magneto, not quite the same dude as the arch-villain to the X-Men.
Although the second season told the origin of Spider-Man, it also took on some drastic cost saving measures by recycling footage from another series "Rocket Robin Hood." Thus, Spider-Man had frequent encounters with unknown aliens and monsters.
Overall, there is a lot of nostalgia for this first Spider-Man series, but among the 6 and counting Spider-Man series that followed this one may have a hard time claiming the title of best.
* The Marvel Super Heroes (1966) * Spider-Man (1967)