Ultra-high molecular weight polyethylene (UHMWPE) has found widespread use as a reinforcement in polymer matrix composites in many ballistic applications due to their desirable mechanical properties such as high modulus, low density, high energy absorption, excellent abrasion, and fatigue resistance. [1][2][3] Additionally, the non-polar, inert, and chemical resistant surface properties allowing the UHMWPE fibers to be biocompatible make them an attractive choice in many medical device applications. However, the inert surface chemistry severely hinders the performance of UHMWPE fiber-reinforced composites in structural applications. [4,5] The performance of composite materials is primarily dependent on the choice of fiber, matrix, and their final properties are typically dictated by the interface between them. [6] Interfacial properties in composite materials are usually determined by chemical interactions, mechanical interlocking, and the size of the surface area between both interface constituents. [7,8] Due to the previously mentioned smooth and chemically inert nature of the fiber surface, interfacial debonding is a common failure mode observed in UHMWPE composites when used in structural applications. The chemically inert surface of the fibers can also result in poor resin wetting of the fibers during composite manufacturing, which can lead to poor interfacial properties. Therefore, it is important to tailor the UHMWPE fiber-matrix interface so that the structural performance of composites can be improved, and their potential applications expanded.To improve the fiber-matrix interface of UHMWPE fiberreinforced polymer composites, researchers have primarily investigated fiber-surface treatments to produce reactive functional groups. Chromic acid [9][10][11][12] and corona discharge [13][14][15][16] treatments are methods that impart micro-pits and introduce functional groups onto the surface of the fibers to improve bonding with the matrix. However, chromic acid treatments and longer corona discharge treatment periods lead to a reduction in the strength of the fiber. Another series of studies have shown that plasma treatments can improve the fiber-matrix interface of UHMWPE fiber-reinforced composites through increasing fiber surface roughness and the introduction of polar functional groups, while preserving the tensile properties. [17][18][19][20][21][22][23] Ultra-high molecular weight polyethylene (UHMWPE) fibers are used in ballistic composites due to their high tenacity; unfortunately, their use in structural composites remains limited due to their poor adhesion with polymer matrix materials. Interphase design to the fiber surface is a promising approach to improve the interfacial properties of composite materials. This work describes the use of an aramid nanofiber (ANF) dip-coating treatment of plasma-treated UHMWPE fibers that increases surface roughness and enhances mechanical interlocking with the matrix. The ANFs also populate the fibers with polar functional groups, specifically hydroxyl, amide, ke...