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Low-dimensional electronic and glassy phononic transport are two importantingredients of highly-efficient thermoelectric material, from which twobranches of the thermoelectric research emerge. One focuses on controllingelectronic transport in the low dimension, while the other on multiscale phononengineering in the bulk. Recent work has benefited much from combining thesetwo approaches, e.g., phonon engineering in low-dimensional materials. Here, wepropose to employ the low-dimensional electronic structure in bulk phonon-glasscrystal as an alternative way to increase the thermoelectric efficiency.Through first-principles electronic structure calculation and classicalmolecular dynamics simulation, we show that the $\pi$-$\pi$ stackingBis-Dithienothiophene molecular crystal is a natural candidate for such anapproach. This is determined by the nature of its chemical bonding. Without anyoptimization of the material parameter, we obtain a maximum room-temperaturefigure of merit, $ZT$, of $1.48$ at optimal doping, thus validating our idea.

Enhancing thermoelectric figure-of-merit by low-dimensional electrical transport in phonon-glass crystals