We have prepared a low-temperature cross-linked soluble polyimide (SPI) as a dielectric material for organic thin-film transistors (OTFTs) to improve their electrical stability. Two types of soluble polyimides (DOCDA/6FHAB and 6FDA/6FHAB) were synthesized by a one-step polymerization process using 5-(2,5-dioxytetrahydrofuryl)-3-methyl-3-cyclohexene-1,2-dicarboxylic anhydride (DOCDA) and hexafluoroisopropylidene diphthalic anhydride (6FDA) as the dianhydrides and 2,2-bis(3-amino-4-hydroxyphenyl)hexafluoropropane (6FHAB) as a diamine. To further enhance the electrical performance, the SPI thin films were crosslinked with methylated/ethylated (hydroxymethyl)benzoguanamine (HMBG) through a low temperature process at 160 °C. Crosslinking considerably improved the insulating properties, resulting in a substantial reduction in leakage current from 10-7 A cm-2 to 10-9 A cm-2 at 2.0 MV cm-1. When crosslinked SPIs were used as gate dielectrics in OTFTs, device stability and reliability, as measured by the off-current, threshold voltage, and hysteresis, improved significantly. Our results demonstrate the potential of crosslinked SPIs as effective gate dielectric materials for advanced organic thin-film transistors.