Transition metal silicides constitute a promising class of inexpensive and non-toxic thermoelectric materials showing competitive properties. This article reports an ef-1 Accepted manuscript / Final version ficient process to synthesize highly textured poly-crystalline CrSi 2 by performing slip casting under a strong magnetic field. The crystallographic texture of spark plasma sintered samples, characterized by electron back-scattered and X-ray diffraction techniques showed a fiber texture symmetry with the c-axis of hexagonal CrSi 2 aligning preferentially along the magnetic field direction. The thermoelectric properties measured both parallel and perpendicular to the c-axis texture direction showed a large anisotropy. In particular, a significantly higher Seebeck coefficient was measured c reaching a maximum value of 200 µV K −1 at 650 K, inducing a power factor c twice higher than ⊥c with an average value of 2.2 mW m −1 K −2 . Density functional theory and transport property calculations revealed that an anisotropic two-band model can explain the higher thermoelectric property along the c-axis direction, which can be traced to Cr-Cr bonding interactions along this direction. The estimated thermoelectric figure of merit ZT c was improved to 0.20 at 773 K. This is 50 % higher than that measured for randomly oriented samples and comparable to that observed for single crystals. Such a performance boost can certainly be reiterated for other types of thermoelectric materials using the efficient magnetic slip-casting process reported in this article.