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Bismuth telluride (Bi2Te3) and its alloys are the best bulk thermoelectricmaterials known today. The stacked quasi-two-dimensional (2D) layers of Bi2Te3were also identified as topological insulators. In this paper we describe amethod for graphene-inspired exfoliation of crystalline bismuth telluride filmswith a thickness of a few atoms. The atomically thin films were suspendedacross trenches in Si/SiO2 substrates, and subjected to detailcharacterization. The presence of the van der Waals gaps allowed us todisassemble Bi2Te3 crystal into its quintuple building blocks - fivemono-atomic sheets consisting of Te(1)-Bi-Te(2)-Bi-Te(1). By altering thethickness and sequence of atomic planes we were able to create designernon-stoichiometric quasi-2D crystalline films, change their composition anddoping, as well as other properties. The exfoliated quintuples and ultra-thinfilms have low thermal conductivity, high electrical conductivity and enhancedthermoelectric properties. The obtained results pave the way for producingstacks of crystalline bismuth telluride quantum wells with the strong spatialconfinement of charge carriers and acoustic phonons for thermoelectric devices.The developed technology for producing free-standing quasi-2D layers ofTe(1)-Bi-Te(2)-Bi-Te(1) creates an impetus for investigation of the topologicalinsulators and their possible practical applications.

From Graphene to Bismuth Telluride: Mechanical Exfoliation of Quasi-2D Crystals for Applications in Thermoelectrics and Topological Insulators