The present study investigates the removal of dichlorvos (DCV) from aqueous environment using a novel Mg-Fe layered double hydroxide (LDH) /montmorillonite (MMT) nanocomposite fabricated with chitosan (Ch), gum ghatti (Gg) and poly lactic acid (PLA). Optimization of parameters was done and maximum DCV removal was noted by LDH/MMT/Ch followed by LDH/MMT/Gg, LDH/MMT and LDH/MMT/PLA with the removal efficiencies of 97.2{\%}, 83.4{\%}, 70.9{\%} and 66.8{\%} respectively. Among the various equilibrium and kinetic models, Freundlich isotherm and pseudo first order showed the best fit indicating the heterogenous mode of adsorption with the involvement of physical forces. Intraparticle diffusion and Boyd plot suggested the film diffusion for all the composites. The endothermic and spontaneous nature of the process was revealed by thermodynamic studies. The mechanism was further elucidated using FT-IR, SEM and EDX analysis. Ex-situ studies showed the maximum removal of 83.1{\%} of DCV from wastewater using LDH/MMT/Ch nanobiocomposite in column mode. Regeneration studies suggested that the adsorbent could be reused up to three cycles.