In this study, inorganic silica nanoparticles are used to manipulate the morphology of 6,13-bis(triisopropylsilylethynyl)-pentacene (TIPS pentacene) thin films and the performance of solution-processed organic thin-film transistors (OTFTs). This approach is taken to control crystal anisotropy, which is the origin of poor consistency in TIPS pentacene based OTFT devices. Thin film active layers are produced by drop-casting mixtures of SiO2 nanoparticles and TIPS pentacene. The resultant drop-cast films yield improved morphological uniformity at ∼10% SiO2 loading, which also leads to a 3-fold increase in average mobility and nearly 4 times reduction in the ratio of measured mobility standard deviation (μStdev) to average mobility (μAvg). Grazing-incidence X-ray diffraction, scanning and transmission electron microscopy as well as polarized optical microscopy are used to investigate the nanoparticle-mediated TIPS pentacene crystallization. The experimental results suggest that the SiO2 nanoparticles mostly aggregate at TIPS pentacene grain boundaries, and 10% nanoparticle concentration effectively reduces the undesirable crystal misorientation without considerably compromising TIPS pentacene crystallinity.