Direct measurements of deuterium main-ion toroidal rotation spanning the linear ohmic to saturated ohmic confinement (LOC-SOC) regime and with additional electron cyclotron heating (ECH) are presented and compared with the more commonly measured impurity (carbon) ion rotation in DIII-D. Main ions carry the bulk of the plasma toroidal momentum, and hence, the shape of the main-ion rotation is more relevant to the study of angular momentum transport in tokamaks. Both in the LOC regime and with ECH, the main-ion toroidal rotation frequency is flat across the profile from the sawtooth region to the plasma separatrix. However, the impurity rotation profile possesses a rotation gradient, with the rotation frequency being lower near the plasma edge, implying a momentum pinch or negative residual stress inferred from the impurity rotation that differs from the main-ion rotation. In the SOC regime, both the main-ion and impurity rotation profiles develop a deeply hollow feature near the midradius while maintaining the offset in the edge rotation, both implying a positive core residual stress. In the radial region where the rotation gradient changes most dramatically, turbulence measurements show that density fluctuations near the trapped electron mode (TEM) scale are higher when the rotation profile is flat and drop significantly when the plasma density is raised and the rotation profile hollows, consistent with instabilities damped by collisions. Linear initial value gyrokinetic simulations with GYRO indicate that the transition from LOC-SOC in DIII-D occurs as TEMs are replaced by ion temperature gradient (ITG) driven modes from the outer radii inwards as the plasma collisionality increases, Zeff decreases, and the power flow through the ion channel progressively increases due to the electron-ion energy exchange. Gyrofluid modeling with trap gyro-Landau fluid (TGLF) successfully reproduces the plasma profiles at key times in the discharge and in time dependent simulations with predictive TRANSP. TGLF indicates that in the LOC and SOC regimes as well as with ECH, subdominant modes are present and that the plasma is not in a pure TEM or ITG binary state, but rather a more subtle mixed state. Predictions of the main-ion rotation profiles are performed with global nonlinear gyrokinetic simulations using GTS and reveal that the flat rotation is due to oscillatory variation of the turbulent residual stress across the profile, whereas the deeply hollow rotation profile is due to a larger-scale, dipole-like stress profile. In these cases, the predicted and observed main-ion rotation profile is consistent with the balance of turbulent residual stress and momentum diffusion.