I'd say yes simply on the fact that Spider-Man is right up there with Mickey Mouse, Superman and Bugs Bunny in name recognition. As for why I'm asking this.
The reason why Disney never gave the show a box set much less an individual release is on the grounds that it probably wouldn't sell well (Their hesitation to release Marvel based DVDs is part of the reason I believe why Marvel has been trying to get the rights back from Disney). First two reasons why I believe Disney was wrong in their decision:
1.Again it's a Spider-Man product.
2. 80s cartoons have been proven to be a success in sales.
And of course Disney would generally release Marvel related DVDs to coincide with the movies (Spider-Man VS Daredevil for Daredevil). That said 2003 would have been the best opportunity for the set for the following reasons:
1. The set would have the advantage of tieing into two Marvel movie franchises:
a. The Spider-Man movie from 2002 and the upcoming movie for 2004.
b. X-Men 2, due to Iceman being part of the main cast and the 4 appearances made by the X-Men (2 cameos, 2 full appearances). Plus Magneto's full appearance and the cameo of The Brotherhood.
2. Since there were also the Daredevil and Hulk movies coming out, they could have advertised the appearances made by those characters (albeit Matt Murdock made the appearance with a cameo of Daredevil). And of course there's the Kingpin's appearance to factor in.