Signal processing over single-layer graphs has become a mainstream tool owing to its power in revealing obscure underlying structures within data signals. For generally, many real-life datasets and systems are characterized by more complex interactions among distinct entities. Such complex interactions may represent multiple levels of interactions that are difficult to be modeled with a single layer graph and can instead be captured by multiple layers of graph connections. Such multilayer/multi-level data structure can be more naturally modeled and captured by a high-dimensional multi-layer network (MLN). This work generalizes traditional graph signal processing (GSP) over multilayer networks for analysis of such multilayer signal features and their interactions. We propose a tensor-based framework of this multilayer network signal processing (M-GSP) in this two-part series. Specially, Part I introduces the fundamentals of M-GSP and studies spectrum properties of MLN Fourier space. We further describe its connections to traditional digital signal processing and GSP. Part II focuses on several major tools within the M-GSP framework for signal processing and data analysis. We provide results to demonstrate the efficacy and benefits of applying multilayer networks and the M-GSP in practical scenarios.