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I am building a scout heavy Dark Angels army, and I want to turn them into fallen. I am curious what others think I could do to give them a good renegade/fallen feel while still sporting the sullen hoods and emblems of the Dark Angels'

Give them the worn down dirty look of renegades that have been fighting for 10K years - perhaps scavenged chaos bits and pieces, perhaps even go for the DA preheresy colour scheme for their armour (black IIRC?).

I have always liked the conversion possibilities of a fallen DA army!

Maybe older marks of armour, less dark angels iconography. Salvaged gear from others chapter/legion perhaps...

There are at least 2 excellent Fallen army threads on DakkaDakka, you should search around a bit.

Since the fluff says they were scattered in place AND time, there should be a wild mix of accessories and states of armour/weapons, where some might look like factory-new pre-heresy DA and others will resemble to the Road Warrior, i.e. very weathered/damaged armour, and salvaged weaponry.

Depending on whether you want them to be just renegade or fallen to chaos, you can throw in parts of CSM and/or xenos parts. For example a few of them might carry (dark) eldar swords or an ork shoota.
You can also go (with all or only a few) the "righteous Fallen" way, putting a lot of incensors, purity seals etc. on them. Those could also go with big banners "Death to the False Emperor" / "Death to the Lion traitor" etc pp.

Scouts are always a good idea in Fallen armies, as a lot of the Calibanite knights were too old to get SM augmentations, and others quit their power armour to blend into different societies.
You could resculpt some of their armour to look a bit more medieval. You should also look for medieval-inspired helmets for power armour. There are some on the DA accessory sprue or in the veteran pack, Maxmini.eu has some others.

(Alternatively or additionally you could for the original DA look - which was Native American style - hence the feathers that can still be found on the stormcannon)

So black armour as a base, some pre-heresy armour & weapons, possibly CSM & xenos parts. Knight helmets, and lots of other bitz that fit.
The more you mix accessories, the more "patched up" they'll look as an army, which is what you want to go for, I guess.