In this study, we prepared and evaluated folic acid-conjugated albumin-paclitaxel (FA-BSA-PTX) nanoparticles using a new green technique, called the high-pressure homogenisation coagulation method (HPHCM). The effect of process parameters such as BSA concentration, coagulant concentration, homogenisation time, homogenisation pressure, water/ethanol ratio, and BSA/PTX ratio was analysed to optimise nanoparticle size, albumin conversion rate, and encapsulation efficiency. BSA concentration was found to exert a great influence on albumin conversion rate and particle size. Meanwhile, the BSA/PTX ratio significantly affected the nanoparticle encapsulation efficiency. Electron microscopy showed that the freeze-dried particles mostly existed in the form of dimers and trimers with an average particle size of 300–400 nm. Infrared spectroscopy indicated that PTX was well encapsulated in BSA. Raman spectra of the synthesised nanoparticles indicated changes in the disulphide bond configuration and protein structure. In vitro drug-release analysis showed that crosslinked nanoparticles exhibited a sustained release. Furthermore, in vitro cell-uptake studies on HeLa cells showed that FA can be used as a targeting ligand for albumin carriers to enhance the active targeting effect of the nanoparticles with a high FR expression. These results suggest that HPHCM is an effective method to prepare FA-BSA-PTX drug-delivery systems.