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What is the best situation to use which vehicle?
Played a game yesterday against Grey Knights and thought I'd get my Hellhound near his troops and flame them like a bosharie, a Cajun pig roast. But, his guys ranked in the hurt with a bunch of plasma and lascanon pain.
Would it have been more wise to let my arty bombard his troops and instead take a DevilDog to melta his own vehicles?

Personally, I prefer the Hellhound by dint of the more versatile weapon (if the Dog isn't hitting the tank, it's wasting a shot, whereas the Hound ignores cover, can multi-glance vehicles if it lines up a good shot, and of course take out infantry nicely). The HH can also be given a multi-melta to add a little AT as well, which is always nice. So Hellhound all the way for me.

I didn't see in the Codex where Hellhounds can take Multi Meltas. Perhaps I'm just blind lol.
They can glance with a flammer? Please excuse me if it's common knowledge; I'm new to the game

The Hellhound's turret flamer (The Inferno Cannon, if I recall correctly) is a S6 weapon, so can glance up to AV12 and penetrate up to AV11 with good rolls. It's far from a perfect weapon for the job, but if there's no infantry in range and you can line the template up over a couple of low-armour tanks, it's far from the worst option. Annoyingly, they can no longer cause an Explodes result, but glances are always good if you have other weapons (such as Autocannons/Multi-lasers) that also do fairly well at glancing and removing HP.