Pollution due to various heavy metals is increasing at an alarming rate. Removal of hexavalent chromium from the environment is a significant and challenging issue due to its toxic effects on the ecosystem. Development of a low-cost adsorbent with better adsorption efficiency is presently required. In this study, waste coconut fibers (CF) were used to prepare its composite with polyaniline (PANI) via in-situ oxidation. The obtained composites with varying loading of PANI (15, 25, 50, and 75%w/w) were characterized by FE-SEM, TGA, and FTIR spectroscopy. The prepared composites were evaluated for their adsorption performance for removal of Cr(VI). It was concluded that the composite with 50% w/w polyaniline loading on coconut fiber exhibited a maximum adsorption efficiency of 93.11% in 30 min. The effect of pH, dosage, and concentration of the aqueous solution of chromium on the Cr(VI) adsorption efficiency of the composite was also studied. From the optimization studies it was observed that the absorbents exhibited the best adsorption response for Cr(VI) removal with 0.25 mg/mL adsorbent at pH 4, in 30 min. The effect of pH, dosage, and concentration of the aqueous solution of chromium on the Cr(VI) adsorption efficiency of the composite was also studied. This study highlights the application of low-cost adsorbent as a potential candidate for the removal of hexavalent chromium. A detailed study on the adsorption kinetics and isothermal analysis was conducted for the removal of Cr(VI) from aqueous solution using coconut fiber-polyaniline composite. From the kinetic investigation, the adsorption was found to follow the pseudo second order model. The data obtained were best fitted to the Elovich model confirming the chemisorption of the Cr(VI) on coconut polymer composites. The analysis of the isothermal models indicated monolayer adsorption based on the Langmuir adsorption model.