Cake layer is considered to play a crucial role in membrane fouling during the coagulation-ultrafiltration process. However, the contribution of the cake layer on membrane fouling and probable natural organic matter (NOM) removal in this process is unclear, leading to a limited understanding of cake layer and potential secondary utilization. Here, ultrafiltration (UF) membrane fouling contribution, NOM removal, and dynamic membrane application of the cake layer were investigated. Results showed reversible fouling was dominated by cake layer, whereas irreversible fouling was determined by both cake layer and residual NOM in coagulation effluent. Compared with direct UF, the cake layer improved approximately by 15 % of HA removal with molecular weight (MW) of 2000–4000 Da. By optimizing membrane material, HA removal and membrane fouling alleviation were synchronously achieved by cake layer deposition-UF. According to mechanisms analysis, HA removal was attributed to the adsorption or interception of HA with larger MW by the cake layer. Zeta potential and fractal dimension of flocs, and contact angle of the cake layer were closely related to HA removal by cake layer, whereas reversible and irreversible fouling were positively correlated with cake layer thickness and floc fractal dimension respectively. Compared with other dynamic membranes, the cake layer had the best economic performance, which provided application potential on NOM removal in micro-polluted surface water.