Methods of sequestering carbon dioxide (CO2) are provided. Aspects of the methods include contacting an aqueous capture liquid, such as an aqueous capture ammonia, with a direct air capture (DAC) generated gaseous source of CO2 under conditions sufficient to produce an aqueous carbonate liquid, such as an aqueous ammonium carbonate. The aqueous carbonate liquid is then combined with a cation source under conditions sufficient to produce a solid CO2 sequestering carbonate. Also provided are systems configured for carrying out the methods.