This study describes the additive manufacturing of 3D polycaprolactone (PCL) scaffolds and their subsequent surface modification using non-thermal plasma technology (NTP) for musculoskeletal applications. 100% interporous scaffolds with porosities ranging from 37 to 66% were manufactured and characterized using scanning electron microscopy (SEM). 2 NTP-based modification strategies were employed: 1) He activation and 2) Acrylic acid NTP polymerization. Gas flow, system pressure and scaffold porosity were systematically varied and their influence on functional group incorporation efficiency and distribution were studied using X-ray Photoelectron Spectroscopy (XPS). The NTP-coated samples with optimal operational parameters were conducted to a series of in-vitro experiments involving MC3T3-E1 osteoblasts and adipose derived mesenchymal stem cells (ADSCs) and the influence on cell adhesion, proliferation and migration was analyzed and compared to untreated and plasma activated samples. The NTP-based acrylic acid coating was found to effectively stimulate cell migration throughout the porous PCL scaffolds for the MC3T3 cells and was also responsible for better ADSC cell adhesion and migration, making them promising structures for musculoskeletal applications.