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Abstract Line intensity mapping (LIM) is emerging as a powerful technique to map the cosmic large-scale structure and to probe cosmology over a wide range of redshifts and spatial scales. We perform Fisher forecasts to determine the optimal design of wide-field ground-based millimeter-wavelength LIM surveys for constraining properties of neutrinos and light relics. We consider measuring the auto-power spectra of several CO rotational lines (from J = 2–1 to J = 6–5) and the [C ii ] fine-structure line in the redshift range of 0.25 < z < 12. We study the constraints with and without interloper lines as a source of noise in our analysis, and for several one-parameter and multiparameter extensions of ΛCDM. We show that LIM surveys deployable this decade, in combination with existing cosmic microwave background (CMB; primary) data, could achieve order-of-magnitude improvements over Planck constraints on N eff and M ν . Compared to next-generation CMB and galaxy surveys, a LIM experiment of this scale could achieve bounds that are a factor of ∼3 better than those forecasted for surveys such as EUCLID (galaxy clustering), and potentially exceed the constraining power of CMB-S4 by a factor of ∼1.5 and ∼3 for N eff and M ν , respectively. We show that the forecasted constraints are not substantially affected when enlarging the parameter space, and additionally demonstrate that such a survey could also be used to measure ΛCDM parameters and the dark energy equation of state exquisitely well.