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Nanofiltration (NF) is increasingly applied for advanced drinking water treatment, but achieving stable operation at high recovery rates remains challenging for surface waters with high scaling potential. This pilot study investigated the performance and optimization of a three-stage NF270 system (4:2:1 tapered array) for treating coagulated surface water in northern Jiangsu, China, aiming to identify sustainable operating conditions for high-recovery applications. The NF system was operated at recoveries of 80–90% with a feed flux of 20–23 LMH, and the effects of forward flushing frequency, acid dosing location, and concentrate recirculation on fouling behavior were evaluated. The NF270 membrane achieved consistent removal of organic matter (effluent chemical oxygen demand (CODMn) < 0.5 mg/L), hardness (40–60% rejection), and alkalinity (~20% rejection), meeting Jiangsu Province drinking water standards. However, operation at 90% recovery resulted in rapid third-stage fouling, with permeate flow declining by >60% within 2.5 h. Osmotic pressure analysis (local concentrate osmotic pressure: 3.8–4.2 bar; net driving pressure: 0.8–2.2 bar) confirmed physical scaling rather than hydraulic limitation as the dominant mechanism. Stage-wise concentration factor calculations (CF1 = 1.6, CF2 = 2.9, CF3 = 4.4) revealed local Langelier Saturation Index (LSI) values of 1.8–2.2 in the third stage, identifying CaCO3 supersaturation as the primary scaling cause. Reducing recovery to 85% and flux to 20 LMH with 2 h forward flushing extended stable operation. Acid addition effectively mitigated scaling, but dosing location was critical: first-stage addition (pH 8.1 → 7.6) reduced third-stage LSI to 0.7–0.9 and stabilized performance, whereas third-stage addition (pH 8.0 → 7.3) inadvertently promoted Al(OH)3 precipitation from residual coagulant (feed Al: 0.07–0.11 mg/L). Concentrate recirculation (90% ratio) did not alleviate fouling. These findings demonstrate that for aluminum-rich coagulated surface waters, optimizing recovery, flushing frequency, and acid dosing location is essential for sustainable NF operation, and provide engineering guidance for full-scale applications.