My personal opinion:
A small company (5-20 people or so) drop it off in person. Shows the initiative and quite likely to meet someone involved in the decision making process.
Medium company follow thier request and hope your resume stands out.
Larger company your SOL no matter how you look at it, with the computer programs screening your information and the hundreds of applicants for a single position your chances are slim. Better home you know someone who can vouch for you and has some pull as you'll need it.
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