2D binary HT-polymers present effective charge transport for both electrons and holes (Table ), with significant tuning by the bridge functionalizations. Specifically, the π-electron density of the 2D skeleton is more distributed at the C=O bridges of CTPAB than that at the CH2 and O brides of MTPAB and OTPAB, respectively. As a result, the structure deformation are less impactive to the wave functions of valence and conduction bands of CTPAB, resulting in smaller DP constants and higher carrier mobilities. The carrier mobility of 2D CTPAB is as high as 6.70 and 0.24 × 10 3 cm 2 V -1 s -1 for electrons and holes respectively, values comparable to those of crystalline silicon (~ 1.40 × 10 3 cm 2 V -1 s -1 ), making this material besides a good photocatalyst candidate for water splitting also a promising 2D organic electronics material.