Thermoelectric materials are attractive in various applications for their ability to convert temperature differences to electrical power via simple electrical junctions with no moving parts. In recent years, particular attention has been paid to thermoelectric materials beyond the usual semiconducting compounds (like $Bi_2Te_3$) in hopes of creating thermoelectric generators that are inexpensive, flexible, and require no rare or toxic elements. 2D materials such as graphene or black phosphorus (BP) could be an ideal solution, and numerous theoretical works have espoused their potential, but so far experimental works have failed to achieve the high performance or scalability needed for practical applications. In this thesis, several research strategies are proposed to solve the current issues of 2D materials in thermoelectric applications through improved exfoliation techniques. These include the production of low-cost BP composite thermoelectric films, synthesis of high-performance n-type graphene, and finally synthesis of p-type graphene to eventually produce all-graphene thermoelectric devise. These results open new avenues of research into 2D materials and represent important progress for the eventual applicability of these materials in real thermoelectric applications.