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Ochratoxin A (OTA) contamination in grape juice has attracted widespread concern as OTA can lead to kidney disease and cause adverse neurological effects. An effective method to remove OTA is to make use of highly adsorbent materials that are able to remove the toxic contaminant. Recently, inactivated Lactobacillus plantarum-based biosorbents have shown to be an efficient, cost-effective and environmentally friendly bioremediation method in removing toxic pollutants such as OTA. We used five chemical thiol-modification methods to improve the adsorption efficiency of OTA in grape juice. The esterification of Lactobacillus plantarum (L-Es) significantly increased the sulfhydryl contents (-SH) by 251.33 μmol/g and >90% of OTA was removed. However, the inactivated microbial adsorbent was difficult to separate after adsorption and therefore, the prepared L-Es were embedded into the cellulose nanocrystals (L-Es@CNCs). Moreover, L-Es@CNCs significantly increased the adsorption rate of OTA in grape juice samples by 88.28% with negligible effects on juice quality due to the properties of easy re-use and excellent biodegradability. This showcases its potential application for OTA removal in the grape juice industry.