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Functionalized carbon nanomaterials are considered to be an efficient modifier for ultrafiltration membranes with enhanced performance. However, most of the reported carbon nanomaterials are derived from unsustainable fossil fuels, while an extra modification is often essential before incorporating the nanomaterials in membranes, thus inevitably increasing the cost and complexity. In this work, novel functionalized biomass-based carbon nanoparticles were prepared successfully from agricultural wastes of corn stalks through simple one-step acid oxidation method. The obtained particles with the size of ~45 nm have excellent dispersibility in both aqueous and dimethyl formamide solutions with abundant oxygen-containing groups and negative potentials, which can endow the polysulfone ultrafiltration membranes with enhanced surface hydrophilicity, larger pore size, more finger-like pores, and lower surface roughness. Therefore, the separation and anti-fouling performance of membranes are improved simultaneously. Meanwhile, the addition of 0.4 wt% nanoparticles was proved to be the best condition for membrane preparation as excess modifiers may lead to particle aggregation and performance recession. It is expected that these biomass-based carbon nanoparticles are potential modifying materials for improving the separation performance and anti-fouling property of the membranes with great simplicity and renewability, which pave a new avenue for membrane modification and agricultural waste utilization.