Cr2+ doped ZnS and ZnSe possess a unique blend of physical, spectroscopic, and technological parameters. These laser materials feature ultra-broadband gain in 1.9 – 3.3 μm mid-IR range, low saturation intensities, and large pump absorption coefficients. The II-VI semiconductor hosts provide a low phonon cut-off, broad IR transparency, and high second and third order nonlinearity. Cr:ZnS and Cr:ZnSe are available in polycrystalline form: the material consists of a multitude of microscopic single-crystal grains with a broad distribution of grain sizes and orientations, which results in random quasi-phase-matching (RQPM). The distinctive features of RQPM are a linear dependence of the conversion yield with length of the medium and ultra-wide bandwidth of three-wave mixing. We review resent experimental results on optically pumped mid-IR ultrafast lasers based on polycrystalline Cr:ZnS and Cr:ZnSe. We demonstrate that Kerrlens mode-locking of polycrystalline Cr:ZnS and Cr:ZnSe lasers allow for generation of few-cycle mid-IR pulses with MW-level peak power. This opens several avenues for efficient nonlinear frequency conversion of short optical pulses directly in the laser gain medium via RQPM process. We implemented Kerr-lens mode-locked Cr:ZnS oscillators, which feature high power (up to 0.25 W), spectrally broad (up to 22 THz) second harmonic generation (SHG) in the laser medium. We also demonstrate simple and robust ultrafast source based on single-pass continuously pumped polycrystalline Cr:ZnS laser amplifier: mid-IR pulses with 6.8 W average power and the spectrum spanning 2.0–2.6 μm as well as SHG pulses with 0.52 W average power and 1.05 – 1.25 μm spectral span were obtained.