All-optical switching (AOS) of magnetization by a single femtosecond laser pulse in Co/Gd based synthetic ferrimagnets is the fastest magnetization switching process. On the other hand, He ion irradiation has become a promising tool for interface engineering of spintronic material platforms, giving rise to significant modification of magnetic properties. In this paper, we explore the use of He ion irradiation to enhance single pulse AOS of Co/Gd bilayer-based synthetic ferrimagnets. The intermixing of the constituent magnetic layers by He ion irradiation was both numerically simulated and experimentally verified. We theoretically modelled the effects of intermixing on AOS using the layered microscopic 3-temperature model and found that AOS ...