In a transition to a circular economy, second‐generation biomass energy has come to the forefront. The present study is aimed at characterizing biochar and byproducts of the pyrolysis of star anise residue (ANI) in the N2 and CO2 atmospheres as well as the kinetics and optimal reaction mechanisms based on the Flynn–Wall–Ozawa and Coats‐Redfern methods. The ANI pyrolysis involved three stages, with the first one (161.5–559.1°C) as the main phase. The activation energy was lower in the N2 atmosphere than in the CO2 atmosphere (179.44–190.17 kJ/mol). The primary volatile products generated during the ANI pyrolysis were small molecule products (H2O, CO2, CO, and CH4), organic acids, alcohols, and ketones. The atmosphere type exerted a minimal impact on the types of gases released, with the CO2 atmosphere increasing CO and CH4 emissions. The pyrolytic oil of ANI contained a variety of organic compounds, including alcohols, phenols, ketones, acids, sugars, and other nitrogen‐ and oxygen‐containing cyclic compounds, with its predominant compounds being acids, esters, ketones, and sugars. The elevated temperature range of 300–700°C enhanced the charring degree of the ANI biochar. The biochar showed stronger aromaticity in the CO2 atmosphere but better granularity in the N2 atmosphere. This study introduced an innovative perspective by showcasing the potential of ANI as a promising biomass source for energy generation and underscored its abundance, sustainability, and applicability as a raw material in fragrance production. It also emphasized the significance of CO2‐reuse technology as a means to mitigate CO2 emissions. The findings of this work offer a theoretical and practical basis for the comprehensive utilization and efficient disposal of star anise residues.