The　Fenton　process　has　been　considered　as　one　of　the　most　promising　advanced　oxidation　processes　(AOPs)　for　the　treatment　of　persistent　organic　pollutants　(POPs).　Herein,　engineered　nanoscale　schwertmannite　(nano–SCH)　were　fabricated　from　a　PVP　(polyvinylpyrrolidone)　assisted　room–temperature　synthesis.　The　as–prepared　well–dispersed　nano–SCH　materials　were　further　studied　as　Fenton–like　catalysts　for　4–nitrophenol　(4–NP)　degradation　in　the　presence　of　H2O2.　Results　showed　that　the　optimized　nano–SCH–0.125　was　able　to　degrade　91.0%　of　4–NP　in　60　min　at　298　K,　thanks　to　the　nanoscale　and　hierarchical　surface　structures　that　provided　abundant　reactive　sites　at　solid/solution　interfaces.　Moreover,　mechanism　study　indicated　that　•OH　radicals　were　the　main　reactive　species　responsible　for　the　excellent　4–NP　degradation　performances　during　the　Fenton–like　processes.　This　work　thus　provides　a　viable　pathway　to　engineer　nanoscale　materials　with　enhanced　catalytic　properties　in　oxidative　degradation　of　environmental　pollutants.　©　2021　Elsevier　B.V.