Although Expanded Talon Company and Talon Outposts Expanded are good enough mods in their own right, I had something more streamlined in mind; something more along the lines of holotapes explaining where they get their stuff, who's that employer who wants the Capital Wastes chaotic, even a little bonus on how they get to outfit their best of the best in Power Armor (preferably T-45d, and merely giving it to them is kind of a stretch).
Armor-wise, the more reinforced versions of combat armor are good enough for a vanilla game, but I'm also thinking of giving them helmets to couple their armor; after all, charging into a battle without your helmet is kind of stupid. Plus, some Metal Armor (and its reinforced variant) would suffice for the more novice of troops, AKA, those who have to earn their colors before being accepted into the Company proper. And like I said before, the best of the best would have Power Armor, but in scarce amounts even then; it'd still be a bit of a stretch, but with a bit of a background story, it'd be preety believable.
Weapon-wise, I'd be more liberal giving them Riot Shotguns, Light Machine Guns, 12.7mm SMGs and the like; seeing as they are one of the most powerful merc companies in the Capital Wastes, I think it'd be not much of a stretch to arm them to the teeth, unlike, you know, Power Armor. Plus, I'd see them having a few gunsmiths here and there to build and maintain all this stuff, so that the Company doesn't fall apart due to lack of weapons. Energy Weapons-wise, though, I'd be somewhat conservative when it comes to that; Laser and Plasma weapons are not as easy to maintain as normal guns, and would as a result be only given to the higher-ups.
Location-wise, I'd see them having a much more fortified Fort Bannister, and many scattered posts near the fort for security reasons. This also makes for much harder fights with them - one of their outposts notices you? Prepare for a world of pain. Outside of Fort Bannister, though, it'd not be absurd of them to have a few bases in Washington DC and other wasteland hotspots, example: near Rivet City and Tenpenny Tower. I'd also imagine them making patrols in routes that connect their outposts and the area surrounding said bases, making for much harder sneaking into them.
Welp, that's all I have here for now.