The magnetic and transport properties of the novel R3T 4As4O2−δ (R = La, Ce, Pr, Nd and Sm, T = Ni and Cu) layered materials were studied using structural and physical properties measurements. Varying the rare-earth ion led to the observation of diverse physical properties including superconductivity for R = La and T = Ni, ferromagnetic or antiferromagnetic order for R = Ce, Pr, and Sm, or spin-glass behavior in Nd3Ni4As4O2−δ. These complex magnetic and electronic properties are discussed in light of the crystalline anisotropy in these layered compounds.