Optical UV–vis and electrical impedance measurements were conducted at room temperature on aqueous solutions with hydroxychloroquine (HCQ) and graphene oxide (GO) molecules. Remarkably, at sufficiently high GO concentration, the HCQ-GO solution exhibited the least loss factor and the Debye relaxation process, suggesting that the polarization of coupled HCQ-GO molecules is cooperative and, hence, correlated within the Debye relaxation time. Indeed, our systematic molecular dynamic calculations of the equilibrium Dipole Auto-Correlation Function (DACF) showed that adding GO enhances the decay relaxation time of DACF for HCQ samples. Moreover, the depression of the characteristic UV absorption peak (at ∼ 342 nm) with increasing GO concentration validated the presence of the HCQ-GO interaction in our samples, agreeing with our calculation based on the simplified time-dependent density functional theory. Our work is, thus, timely regarding the current high demand for a method to remove HCQ from the aqueous environment. It is also relevant to drug delivery applications considering the anticancer efficacy of HCQ and the biocompatible GO as a potential drug carrier.