FOR FUTURE REFERENCE FOR ME...:]
Unlock Pichu:
Complete Legendary Pokemon Event 37 and defeat Pitchu when he challenges you.
Unlock Dr. Mario:
Complete Classic in 1-P mode using Mario with any difficulty and without continuing.
Unlock Jigglypuff:
Complete Adventure or Classic in 1-P mode in any difficulty.
Unlock Mewto:
Complete 20 hours of combined Vs Time total then defeat Mewto when he challenges you.
Unlock Luigi:
Complete Adventure mode with a 2 in the seconds metre like for example; 04:32:34. You will then view a scene where Luigi kicks Mario away so he can fight you with Peach. Defeat them both to unlock Luigi then Defeat Luigi.
Alternate Character Unlocks
Unlock characters by playing a certain number of vs. Matches.
Jigglypuff:
50 vs. Matches
Dr. Mario:
100 vs. Matches
Pichu:
200 vs. Matches
Falco:
300 vs. Matches
Marth:
400 vs. Matches
Young Link:
500 vs. Matches
Ganondorf:
600 vs. Matches
Mewtwo:
700 vs. Matches
Luigi:
800 vs. Matches
Roy:
900 vs. Matches
Mr. Game & Watch:
1,000 vs. Matches
Aiku Saramna Community Member 
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Community Member