In perovskite solar cells (PSCs), the electron transfer layer (ETL) characteristics have significant effects on the photoelectric conversion efficiency (PCE) of the devices. Herein, a natural chelating agent polymer polyaspartic acid (PASP) is doped into the SnO2 precursor solution attributed to a strong interaction between PASP molecules and SnO2, which strengthens the interface contact and passivates the vacancy oxygen trap of the obtained SnO2 ETL, thus promoting the transfer of electrons. In addition, PASP can also regulate the growth of perovskite crystals, leading to an improved crystal quality of the perovskite films. Meanwhile, there is an excellent chelate anchoring of PASP to uncoordinated Pb2+, facilitating the reduction of trap defects at the interface, improving the stability of device, and suppressing the leakage of toxic Pb. Finally, the photovoltaic performance of the optimized device was greatly improved, and the PCE was increased from 21.22 to 23.49%, with outstanding environmental stability. This work provides an inexpensive and efficient treatment strategy that improves the performance and stability of friendly environmental PSCs.