Sulfate radical (SO4•−)-based advanced oxidation processes (SR-AOPs) have been studied to date by utilizing metal–organic frameworks as efficient catalysts to generate sulfate radicals by peroxymonosulfate (PMS) activation in water purification. It is important to select high-performance and reliable catalysts for efficient water remediation, and separation and recovery of catalysts are essential in the practical application of MOFs. Herein, we adapted thermally curable, shape-controllable, and cost-effective agarose (AG) as a smart matrix and ZIF-67, as a powerful catalyst to prepare nanoarchitectured aerogel (Z67@AG). This nanoporous aerogel composite can efficiently generate sulfate radicals and hydroxyl radicals by activating PMS in the nanopores. Z67@AG aerogel could be easily fabricated in various molds to make desired shapes. This approach enables its utilization for different filtering systems and demonstrates cost-effective and stable performance by mass production and reusability. In the SR-AOP, aerogel exhibited excellent catalytic decomposition performances of 95 % and 88 % efficiencies within 8 and 10 min for dye and levofloxacin, respectively. It is believed that the proposed highly catalytic nanoporous aerogel nanocomposite having cost-effectiveness, excellent catalytic activity, facile fabrication of desired shapes, and an excellent porous structure can be extended to the synthesis of various nanocomposites and emerging applications.