Metal-Organic Frameworks (MOFs) are increasingly being applied in space, automotive, electronic and aerospace applications. In this chapter, high performance engineering polymeric fibres are demonstrated to not only reinforce low melting metals and alloys due to their superior mechanical properties, high thermal resistance up to about 650 °C and resistance to corrosive environment but also light weight resulting composites by reducing the densities. High-performance polymer fibres have superior mechanical properties like specific strength and stiffness that enable them for structural applications. Though high-performance polymer fibres like Kevlar and Zylon were developed two to three decades back, they were still not used as a reinforcement in metal matrix composites, but were used only with other polymer matrices, which generally have good wettability and low processing temperature which are sufficiently low enough not to degrade the reinforcing polymers but also provide cost effective product level solutions with superior performance. Some of the reasons for not using high-performance polymer fibres as a potential reinforcement in metallic materials are their low wettability, poor interfacial properties, and low degradation or heat distortion temperatures in relation to the metal matrix, when processed by conventional manufacturing processes. This chapter presents techniques of metallizing the high-performance polymer fibre surfaces for compatibility with the metallic matrices, using techniques such as electroless coatings, Radio Frequency (RF) ion sputtering and High Velocity Oxygen Fuel (HVOF) thermal spray processes. The metallic coatings improve the wettability of the polymer fibre with the metal matrix and protect the fibre from high thermal gradients that arise during