Here, tuning of the optical properties of emission centers by tailoring the ligand fields is investigated. Experimentally it is demonstrated that Ni2+ can act as a single emission species in multiple-octahedral local environments. Nanocrystal-embedded hybrid materials are employed as hosts in order to take advantage of their convenience in local environment design for practical applications. Novel composite gain materials with high transparence are successfully made, and show interesting wavelength-tunable and ultra-broadband infrared luminescence covering the whole near-infrared region from 1100 to 1800 nm. The infrared luminescence peak positions can be finely tuned from 1300 to 1450 and to 1570 nm, with the largest full width at half maximum being about 400 nm and covering the telecommunication bands at 1200-1500 nm. According to the results of characterization, the unusual luminescence, interestingly, originates from Ni2+ in nanocrystals and the doping efficiency of N2+ is surprisingly high. The results demonstrate that the method presented may be an effective way to fabricate multifunctional light sources with various fundamental multifunctional applications from efficient broadband optical amplifiers to bio-imaging