I actually nearly only use Syrinscape improvisation style. I accomplish this by a few factors:
I listen to the soundsets a lot - Surfing the net? Writing something? Washing the dishes? Tidying up the house? Organizing your bookshelf? I play a soundset I haven’t listened to in a while, and change the moods every few minutes. That way I gradually become familiar with various sets. This is probably the most useful thing I’ve done, because I often find sounds in sets that might not seem immediately relevant to my current campaigns, but end up being useful later, or find something I can recommend to a GM who does need them. Or else I find sounds that can be used for more than one thing: I once needed a sound like someone constantly cracking twigs, and I realized that the “fireplace” sound from Friendly Tavern, turned down low enough that the flame roar couldn’t be heard, just the snap of the flames, sounded just like cracking twigs.
I use the Campaigns feature - If my characters are going to be in forest or desert, dungeon or city, I can pull up the correct campaign to have the most appropriate sets very close at hand.
I am the Dungeon Master - Generally I have an idea of where my players are going, what they’re going to be fighting, and who they’ll be encountering during any given session (even though I usually look up monsters about 10 minutes beforehand). Even if they have several possible courses of action, several possible monsters to fight, several places to go, there is no place they’re going, no monster they’re fighting, no person they’re talking to that I am not in control of. And if they do something completely off the wall, totally unexpected, somehow teleport from the Desert Tomb of the Sun Pharaoh to an Abandoned Spaceship in the Barrier Peaks, tell them it’s time for a ten minute break so you can reset, because that’s fair for everyone. You don’t have run your session like it’s professionally scripted series! It’s ok to have a few pauses while you grab a quick change of music or turn off part of the fight that’s no longer needed.
Build Custom Moods in Obvious Places for You - If I know they’re likely to go to someplace that requires a custom mood often, I usually build that mood and save it, not in the Custom Mood set, but in a similar set that I will reference often. If I needed a variation on a town, for example, I might save a custom mood in Brindle Town rather than one of the Custom Mood sets, because then I know all “town” sets are in the same place. That usually leads to less clicking around.