The potential energy surfaces for ClCS dissociation into ClCS + Cl in the five lowest electronic states have been determined with the combined complete active space self-consistent field (CASSCF) and MR-CI method. The wavelength-dependent photodissociation dynamics of Cl2CS have been characterized through computed potential energy surfaces, surface crossing points, and CASSCF molecular dynamics calculations. Irradiation of the Cl2CS molecules at 360-450 nm does not provide sufficient internal energy to overcome the barrier on S, dissociation, and the S-1/T-2 intersection region is energetically inaccessible at this wavelength region; therefore, S-1 --> T-1 intersystem crossing is the dominant process, which is the main reason S-1-S-0 fluorescence breaks off at excess energies of 3484-9284 cm(-1). Also, the S-1 --> T-2 intersystem crossing process can take place via the S-1 - T-2 vibronic interaction in this range of excess energies, which is mainly responsible for the quantum beats observed in the S-1 emission. Both, direct dissociation and S-1 - S-3 internal conversion are responsible for the abrupt breakoff of S-2 - S-0 fluorescence at higher excess energies. S-2 direct dissociation leads to the formation of the fragments of Cl((X) over tilde P-2) + ClCS((A) over tilde (2)A") in excited electronic states, while S-2 --> S-3 internal conversion followed by direct internal conversion to the ground electronic state results in the fragments produced in the ground state.