Contamination of water by heavy metals is a major environmental concern due to the potential ecological impact on human health and aquatic ecosystems. In this work, we studied the chemical modification of various fruit peels such as banana (BP), granadilla (GP), and orange ones (OP) in order to obtain novel bio-adsorbents to improve the removal of Zn(II) ions from 50 mg·L−1 synthetic aqueous solutions. For this purpose, sodium hydroxide and calcium acetate were employed to modify the fruit peels. The moisture, extractives, lignin, hemicellulose, and cellulose contents of the raw materials were determined according to ASTM standards. The obtained bio-adsorbents were characterized by scanning electron microscopy (SEM), Fourier Transform Infrared Spectroscopy (FTIR) and thermogravimetric analysis (TGA). The results showed the OP bio-adsorbents performed better, especially when the concentration of the modifier solutions increased, e.g., the OP particles modified using 0.8 M NaOH and Ca(CH3COO)2 solutions resulted in 97% removal of Zn(II) contaminating ions and reached a maximum adsorption capacity of 27.5 mg Zn per gram of bio-adsorbent. The adsorption processes were found to follow a pseudo-second order model. The error function sum of square error indicated the Freundlich isotherm (non-linear regression) as best fit model. The obtained results are particularly interesting for material selection in wastewater treatment technologies based on contaminant adsorption.