Nonlinear optical (NLO) properties allow the engineering of a variety of optical devices like organic light-emitting diodes, field effect transistors, and optical sensors, being promissory in fields like telecommunications and electronic engineering, for instance. In opposition to common inorganic chromophores, organic dyes are advantageous once they better resist the breakdown stresses caused by high-power lasers, besides functionalizing diverse circuits with pronounced packaging and miniaturization capabilities. Due to these potentialities, we have experienced a great discussion about how to tune and improve the NLO of organic chromophores. In this direction, besides usual chemical synthesis, proton scavenging procedures can modulate the ONL response of some dyes over a wide range of values. Considering all aspects presented above and attempting to understand these effects, we discuss how the association of solute-solvent interactions and proton remotion can affect two popular dyes, methyl orange, and p-coumaric acid.