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I was always terrible at setting Gambits in FFXII. Like, really bad. I don't know when or even if I'll pick up FFXII: TZA but if I do then I'm relying on you guys to help me get good. So, when you do get the game, let me know which Gambits make you go "Hallelujah!".
Foe: Fire-weak - Fire/Fira/Firaga
Foe: Ice-weak - Blizzard/Blizzara/Blizzaga
Foe: Thunder-weak - Thunder/Thundara/Thundaga
Foe: Wind-weak - Aero/Aeroga
Healing ones are essential. Obviously attack ones. I fiddle w/ mine throughout the game, & will add ones like Karifean mentioned when I think they'll be necessary.
Enemy HP is 100% = Steal
For a mage, Karifean's set is invaluable. The Foe: 100% = Steal gambit is very useful for your lead character. You'll generally want to include a Foe: Flying = [x] in there when you start encountering flying enemies with greater regularity. The x can be anything from magic or a thrown item, but you get telekinesis really late in the game unless they've changed that and of course, with the job system not everyone might have offensive magick.
But the general pattern of healing, support, attack works well. You'll want your revival options first, followed by one or two healing gambits, possibly arranged like so:
Ally: KO = Phoenix Down/Raise
Ally: <30% HP = Cura
Ally: <50% HP = Cure
Or something like that. A general healing gambit, but supplanted by an 'oh smurf I need healing NOW' gambit with lower HP. Remember though cure now has an AoE, which is useful.
Essential support buffs like Haste, Bubble and Protect come next so they can be cast mid-battle, followed by an attack gambit or two. The attack gambits will obviously vary. For a mage, the 'elemental weakness' set is great, while physical fighters can probably get away with a more basic attack command, though feel free to experiment with all the different ones. I sometimes like to activate one that targets the enemies with the lowest HP, which is great in mob fights.
Of course the great thing is you're given all the gambits when you unlock the system. I had to wait forever to get the elemental weaknesses.
No need to care too much about flying opponents since you'll likely run a couple party members with ranged weapons anyways - Uhlan, Monk, Machinist, Archer, Time Battlemage, and of course offensive magic through the Black Mage or Red Battlemage. And I don't remember a single flying opponent tough enough to require more than one party member attacking it (maybe Garuda or Bloodwing if you're underleveled for them).
Something very important to keep in mind with gambits though is that they won't activate if the game deems the action pointless even if the condition is fulfilled.
Ally: any - Phoenix Down
will ONLY activate on KO'd party members anyways. So no need to go out of your way to buy and set up Ally: KO instead. Also you can have this gambit on all of your party members, they will coordinate and won't use more than 1 Phoenix Down per downed party member. However, if you have a White Mage you may want to turn everyone else's revival gambits to the White Mage only so you don't waste Phoenix Downs and just let the White Mage's revive everyone else with the Raise spell.
Oh, my personal favorite attacking gambit is
Foe: Lowest HP - Attack
I don't remember a single part in the entire game where I'd rather go against it. But if there is, you can always just turn off gambits and set your target manually, or put a "Foe: Party leader's target - Attack" gambit on higher priority.
Late in the game I'm also always a fan of
Ally: Party Leader - Hastega/Protectga/Shellga
Unlike other buffing gambits this one allows you to control and make sure all your party members are actually hit by your ga buffs =P
Two more tips: if you have MP issues, either set yourself up with a Charge gambit (great way to restore MP if you're very low on it) or use Syphon on your attacking party members. They won't be needing their MP and if they're not in Shell it's a surefire way to drain all their MP to your mage in one turn. If they are in Shell status it may miss, so beware.
Oh yeah I forgot Ally: Any is a surprisingly versatile gambit.
Having an MP: <10% = Charge gambit is useful for spellcasters. I recommend 10% because Charge's failure rate gets higher the more MP you have.