You need to do this very early in the game and its not likely to succeed. They are your natural enemies. Are you at war with another faction that has an alliance with them or vice versa. If so your relations will drop over time and it may not be possible for an alliance. You will also need a very high global rep to maintain the alliance.
Consider a marriage proposal with them. This will provide an automatic alliance and greatly improve your relations with them. You need to plan ahead to do this though and keep rejecting suitors offered for heir/FL at start of each turn until you spot a suitable Spanish princess preferably with 4+ hearts. And/Or use your princess to marry into them if possible. Marriage alliances are generally stronger and likely to hold longer. Multiple marriages is better still.
Normally with an alliance your relations should improve slightly every turn so there shouldn't really be a need to gift unless you need a quick boost. Its generally a good idea to exchange access rights with any faction you have allied. If you don't then your relations will drop quickly if either cross into each others territories.
Spying/bribing or assassinating damages relations and in some cases rep.
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