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Sure, you can headshot someone with a sniper rifle if you happen to be carrying one - but can you do that the second you see a dual needler whore, and not let him fill you with needles first?
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yes
Best combo in my opinion, and many others, is Battle Rifle + Plasma Pistol.
Charged Shot, switch to BR, and you can literally kill anyone in a split second. It's even more usefull because it can easily take down Overshields.
Best magnum combos would be SMG + Mag or Mag + Plasma Pistol