Abstract: Atomically thin van der Waals materials provide a versatile and unique platform for exploring novel physical interactions at low dimensionality and enabling new device geometries with tunable functionalities. In this talk, I will mainly focus on our recent progress on 2D magnetic materials and low-dimensional magnetic molecules. The first part will include our most recent work on 2D AFM transition-metal phosphorous trichalcogenides, where we couple the magnetic transitions into the mechanical degree of freedom. We observed the expected steady-state spin transitions based on magnetostriction effects and saw signatures of additional transitions arising from magnetic domain dynamics, with magnetic tuning effects of mechanical nonlinearity. I will then present the results on spin-polarized light-emitting diodes made from 2D magnetic/semiconductor heterostructure, which achieve electrical tunability of the emitted light chirality. The last part focuses on the organic 2D molecular system with bistable spin transitions. I will discuss the fabrication, integration with other 2D systems, and the identification of layer-dependent spin-crossover transitions with optical spectroscopies and optomechanical approach.