This article reports on a new class of stimuli-responsive surfactant generated from commercially available amPhiphiles Such as,dodecyltrimethylarrunmohium bromide (DTAB) by substitution of the halide counterion with counterions such as 2-cyanopyrrolide, L-ptolirie that complex reversibly with CO2,. Through a combination of small-angle neutron scattering (SANS), electrical conductivity measurements, thermal gravimetrit analysis, and molecular dynamics simulations, we show how Small changes in charge reorganization aria counterion, shape and size induced by complexation with CO2, allOw for fine-tunability of surfactant properties. We then use these findings to demonstrate, a range of potential practical uses, from manipulating microemulsion droplet morphology to controlling micellar and vesicular aggregation. In particular, we focus on the binding of these surfactants to DNA and the reversible compaction of 'surfactant DNA complexes upon alternate bubbling of the solution with CO2 and N-2.