An unpredictable rise in greenhouse gas (GHG) emissions is a primary concern to the global scientific community. It is directly related to the rapid expansion of the human population and associated with the immense energy demand. The combustion of hydrocarbon fuels in internal combustion (IC) engines releases a large amount of carbon dioxide (CO2), which is one of the causes of GHG emissions. Mitigation of CO2 emissions is a significant challenge to the world. Although several researchers have focused on capturing CO2 from power plants, some researchers have taken initiatives in recent times to capture CO2 in IC engines. This study particularly explored the possibility of using a biomass based‐adsorbent to capture CO2 in the exhaust of a diesel engine. Initially, activated carbon was obtained from palm shells by adopting the preparation methods such as (i) carbonization and (ii) chemical activation. Then, the produced activated carbon was analyzed to examine its physicochemical characteristics and surface textural properties by adopting characterization techniques. The adsorbent sample was loaded in an in‐house fabricated adsorption chamber which was attached to the exhaust of a single‐cylinder, four‐stroke, naturally aspirated, air‐cooled, direct injection (DI), constant speed diesel test engine. The performance of palm shell‐based activated carbon was evaluated as a potential adsorbent for CO2 capture when the engine was operated with two distinct fuels, (i) 100% diesel (D100) and (ii) an optimum biodiesel‐diesel blend (JME20) comprising 80% D100 and 20% Jatropha Methyl Ester (JME). The experimental results showed that an average of about 30% and 37% of CO2 was captured by using palm shell‐based adsorbent in D100 and JME 20 operations, respectively.