Global warming, primarily driven by emissions of greenhouse gases, particularly carbon dioxide, has emerged as a widely acknowledged concern. Hence, the development of novel carbon capture materials with high capacity and low cost holds substantial practical significance. This study investigates the influence of aging time, pH, and copper salt on the synthesis of Cu2(OH)PO4 and its CO2 adsorption performance. Cu2(OH)PO4 adsorbents were synthesized under various aging time, pH, and copper salt conditions, and their morphology and surface functional groups were characterized. Experimental findings indicate that excessively prolonged or abbreviated aging times adversely affect the formation of distinct, discernible lamellar structures within the material. Different pH levels influence the stacking configuration of the lamellae, impacting both their thickness and size. Under acidic conditions, lamellae exhibit dispersed three-dimensional stacking; under neutral conditions, lamellae notably enlarge and demonstrate two-dimensional stacking; at pH 9, lamellae stack three-dimensionally and aggregate. Additionally, the CO2 adsorption performance of Cu2(OH)PO4 adsorbents synthesized with different copper salts varies. By examining the relationship between surface functional group content and CO2 adsorption capacity, we deduced the mechanism by which various synthesis conditions affect both surface functional groups and adsorption capacity. Cu2(OH)PO4 synthesized with a 24 h aging time, pH 7, and CuSO4 as the copper salt exhibits the highest CO2 adsorption capacity, achieving 1.006 mmol/g.