Biological air pollution control is gaining attention as a sustainable alternative for treating CO2-rich gas streams. This study evaluated a trickle-bed photobioreactor with immobilized Chlorella vulgaris UTEX 2714 for biological CO2 removal. Microalgal biomass was encapsulated in sodium alginate capsules, providing approximately 100 g TS/dm3 of active biomass, and the reactor was supplied with ambient air enriched with technical-grade CO2 to 25% v/v. The tests were conducted for 60 days in 20-day operating cycles, under controlled illumination and monitored pH and temperature conditions, and CO2 concentration was determined by means of gas chromatography with a thermal conductivity detector. CO2 removal depended strongly on gas volume flux. At 25 dm3/h, removal efficiency reached 39.9%, corresponding to 117.4 g CO2/day, whereas at 200 dm3/h, it decreased to 5.9% because of the shorter gas–biomass contact time. The immobilized system enabled markedly higher biomass density than conventional suspended-growth photobioreactors, where typical C. vulgaris cultures reach substantially lower biomass concentrations; as a reference, suspended C. vulgaris supplied with desulphurized real exhaust gases produced 2120 ± 123 mg VS/L and achieved CO2 utilization efficiency of 41.4%. A preliminary energy estimate indicated that artificial red/blue LED illumination would require approximately 100 W per module, giving a cost-magnitude energy demand of about 20 kWh/kg CO2 removed under fully artificial 24 h lighting; this demand could be reduced by hybrid sunlight–LED operation. The results indicate that immobilized microalgae can enhance CO2 biosequestration by increasing biomass density and improving gas–biomass contact. However, because effective treatment was achieved mainly at low gas flow rates, the technology should be regarded as suitable for small-to-medium, high-concentration CO2 sources, such as biogas upgrading units or selected industrial kilns and furnaces, rather than the main flue gas stacks of large power plants.