We used density functional theory to calculate the angular resolution anisotropic charge mobility of the substituted chrysene molecules, viz, 4,10-diphenoxychrysene (DPC), 4,10-bis(phenylsulfanyl)chrysene (BPSC), and ethyl 8,9,12-trimethoxychrysene-6-carboxylate (ETCC). The highest occupied molecular orbital-lowest unoccupied molecular orbital gap for DPC, BPSC, and ETCC was calculated to be 3.92, 3.83, and 3.81 eV, respectively, which inferred the compounds to be wide-band-gap semiconductors indicating that the compounds should have high stability in atmospheric conditions. The fact is also supported by electronic band-structure calculation. In addition, higher electron affinity of studied compounds as compared with the bare chrysene molecule imparts enhancement of n-type character in the compounds. The maximum hole ( h Φ ) and electron mobilities ( e Φ ) for DPC compound were found to be 0.739 cm 2 V −1 s −1 and 0.319 cm 2 V −1 s −1 , respectively, at Φ = 0 • . On the other hand, in the case of BPSC crystal, comparatively larger anisotropic electron mobility (0.709 cm 2 V −1 s −1 at Φ = 0 • and Φ = 179.90 • ) than the hole mobility (0.208 cm 2 V −1 s −1 at Φ = 127.19 • and Φ = 307.10 • ) was noted. Similarly, in ETCC, the parallel dimers were found to contribute maximum h Φ and e Φ of 0.052 and 0.102 cm 2 V −1 s −1 , respectively, at Φ = 0 • . The substitution of -SPh in BPSC and -OCH 3 and -CO 2 CH 2 CH 3 in ETCC have relatively more impact on band reduction than -OPh in DPC, thus facilitating electron transport in BPSC and ETCC.