A new magnetically recoverable silica-based nickel(II) nanocatalyst was synthesized by a simple cost-effective procedure, which was characterized by TEM, SEM, XRD, VSM analysis, and FT-IR spectrophotometry. The catalytic activity of the prepared Ni(II) nanocatalyst was tested in two complementary reactions: C-N Chan-Lam cross-coupling of phenylboronic acid with aryl amines and C-C Suzuki-Miyaura cross-coupling reaction of phenylboronic acid with aryl halides. The catalyst was easily recovered by magnetic separation and reused for five times. It demonstrated better catalytic activity in the C-N Chan-Lam reaction compared to C-C Suzuki-Miyaura reaction. Ease of recovery and reusability up to five cycles without noticeable loss of performance in the C-N cross-coupling reaction make the present protocol beneficial both industrially and environmentally. In this paper, a new magnetically recoverable silica-based nickel(II) nanocatalyst was synthesized and applied in two complementary reactions: C-C Suzuki-Miyaura reaction and C-N Chan-Lam reaction. The difference in catalytic activity makes it possible to use this catalyst for cases that are prone to both reactions and selectively create the desired product.