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With a '2 barrel' TBI setup, is it possible to tune this to run with only a single injector running at low load, then at high load, bring on the 2 second injector, just like a carb opening up back in the day?

I am running a TBI on a 4 cylinder and I think it is going to be too much fuel except under high load conditions.

Can this be done, or is there a better way to accomplish the fueling I need?

The computer will allow you to program the required amount of fuel for the quantity of air going in. You wont need to 'switch on' the second injector to achieve what you want. Details will be specific to the computer your running. You will also be able to configure 'power enrichment' (may be named differently depending on computer type) which achieves fine grained control over the extra fuel delivered when you hit the throttle. Essentially you can do achieve the same as a carbie with the computer and also more depending how deep you want to go. Mostly though sticking with the factory tune and only making fewer changes for your engine gives you this for minimal work.