Provided herein are polyethylene compositions with broad orthogonal composition distribution. The polyethylene compositions may comprise at least 65 wt % ethylene-derived units and from 0 to 35 wt % of C3 to C12 olefin comonomer-derived units, and furthermore may exhibit a reversed comonomer index (RCI,m) of 100 kg/mol or greater, a Tw1-Tw2 value of from −16 to −38° C., and an Mw1/Mw2 value of at least 0.9, such as 0.9 to 4. Also provided are processes for making the polyethylene compositions, as well as films made from the polyethylene compositions. Such films may feature superior film stiffness for a given polyethylene composition density, and accordingly such films in some embodiments have average MD/TD modulus and density satisfying the following equation: Avg. Modulus≥1.2*(C1*Density−C2), where C1 and C2 are constants, such as C1=2,065,292 and C2=1,872,345.