This thesis investigates the influence of depletion-driven attractive interactions in quasi-two-dimensional buckled colloidal monolayers on a triangular lattice. Without depletion, such that the interparticle interactions are hard-sphere-like, this experimental system is known to exhibit behaviors akin to a geometrically frustrated Ising antiferromagnet. The present research explores the effects that arise when a short-range attractive interaction (depletion attraction) between particles is introduced. We demonstrate that the added depletion attraction can influence both the magnitude and the sign of the Ising spin coupling constant. As a result, the nearest neighbor Ising spin'' interactions can be characterized as antiferromagnetic, paramagnetic, or ferromagnetic. We compute the effective Ising nearest-neighbor coupling ($J/k_BT$) using a simple theoretical model; the model shows that a competition between entropic effects can modify the sign of the coupling constant from negative to positive and passing through zero. In experiments, the depletion interactions are induced by surfactant micelles comprised of hexaethylene glycol monododecyl ether ($\text{C}_{12}\text{E}_{6}$); these rod-like micelles change length with increasing temperature and offer means to tune the depletion attraction $\textit{in-situ}$ by utilizing temperature-tunable shape anisotropy. The experiments demonstrate the crossover behavior from Ising antiferromagnetic to paramagnetic in the buckled colloidal suspension as a function of depletion attraction. Additionally, spin-flip temporal autocorrelation functions are measured. The correlation functions exhibit both exponential and glassy dynamics. The glassy dynamics are driven by different underlying mechanisms and are observed in the negative and positive coupling-constant regimes. In total, this thesis introduces novel colloidal matter with complex dynamics and magnetic'' features that are rarely observed in traditional atomic systems.