They're large and nearly full-grown. So they'll "escape" the effects of anything you spray.

Effective management at this stage includes one or more of the following:
-- search-and-destroy missions
-- drown in slightly soapy water
-- feed them to the birds/chickens
-- snip in half

Chop sticks are good at grabbing them and then, yes put them in a non-green area so birds feast on their rotten defoliating carcases. I promise I'm not spiteful.

Those are tobacco hornworms, in case you don't know. They are the primary caterpillar pest of tomatoes in many locations. They can be picked up and removed by hand. I often toss caterpillars into the bird bath, which results in a noisy free-for-all for the lucky birds.