Abstract The susceptibility of nickel-based superalloys to processing-induced crack formation during laser powder-bed additive manufacturing is studied. Twelve different alloys—some of existing (heritage) type but also other newly-designed ones—are considered. A strong inter-dependence of alloy composition and processability is demonstrated. Stereological procedures are developed to enable the two dominant defect types found—solidification cracks and solid-state ductility dip cracks—to be distinguished and quantified. Differential scanning calorimetry, creep stress relaxation tests at 1000 °C and measurements of tensile ductility at 800 °C are used to interpret the effects of alloy composition. A model for solid-state cracking is proposed, based on an incapacity to relax the thermal stress arising from constrained differential thermal contraction; its development is supported by experimental measurements using a constrained bar cooling test. A modified solidification cracking criterion is proposed based upon solidification range but including also a contribution from the stress relaxation effect. This work provides fundamental insights into the role of composition on the additive manufacturability of these materials.