The present invention provides a method of preparing mimicking angiogenic co-spheroids, comprises: co-cultring a neural related cell and a cultured cell on hyaluronan-grafted chitosan (CS-HA) substrates to form a co-spheroid of neural related cell/ cultured cell, and encapsulating the co-spheroid of neural related cell/ cultured cell into a hydrogel to form a mimicking angiogenic co-spheroid. The mimicking angiogenic co-spheroid of the present invention can be formed by 3D printing model as a 3D mini-neurovascular unit, which is applicated to a high-throughput angiogenesis screening platform.本發明提供一種製造模擬血管新生的細胞球的方法,包含:在幾丁聚醣-透明質酸(CS-HA)薄膜上共培養神經相關細胞及培養細胞以形成神經相關細胞/培養細胞之細胞球,進一步將神經相關細胞/培養細胞之細胞球包覆至水膠中以形成模擬血管新生的細胞球。本發明可結合3D生物列印方法形成模擬血管新生的細胞球作為微型神經血管單元,其可應用於高通量血管新生藥物篩選平台之用途。