To overcome the precision limitation and environmental impact of current chemical-based production methods for manufacturing silk microfibres used for targeted drug delivery, this paper presents a high-precision, scalable, eco-friendly mechanical machining approach to produce such microfibres in the form of discontinuous chips obtained through elliptical vibration turning of silk fibroin film using a diamond tool. The length and waist width of fabricated microfibres can be precisely controlled. As each vibration cycle will produce one silk microfibre, complete and deterministic chip breakage becomes an essential and challenging task in this approach due to its unique two-phase structure. Thus, the hybrid FE-SPH numerical simulations and machining experiments were conducted to gain a pioneering and in-depth exploration of the chip-breaking mechanism in this process. It was found that applying a low depth ratio (ratio of the nominal depth of cut to the tool path vertical amplitude) and a high horizontal speed ratio (the nominal cutting speed versus the critical workpiece velocity) could effectively reduce the average tool velocity angle (the angle from the deepest cut to the tool exit point along the cutting direction). A smaller angle would enhance the diamond tool's shearing action and led to the reduction of hydrostatic pressure in the cutting zone and a consequent decrease in the ductility of silk fibroin due to its unique structure dominated by beta-sheet crystallites. The above adjustments collectively facilitated chip breakage. This paper, therefore, established a governing rule for the controlled and repeatable formation of microfibres based on the average tool velocity angle for the first time and revealed that the cutting chips would undergo complete and deterministic breakages once the angle approached below 22.6°. On this basis, the high-precision and scalable manufacturing of silk microfibres with precisely controllable length and waist width was ultimately achieved.