Custom tailoring of HELP matrix properties. a) HELP schematic illustrating specification of the RGD ligand concentration by blending different ELP variants in the material. b) HELP schematic illustrating that matrix stiffness is precisely modulated by changing the number of crosslinks (top), while matrix viscoelasticity is tuned by replacing benzaldehyde with aldehyde moieties. c) Shear storage moduli of Stiff Elastic (EL) and Soft EL HELP formulations. Student's t‐test, ** = p < 0.01, N = 3–5. d) Step‐strain–stress relaxation curves comparing EL formulations. e) Cross‐sectional area measurements of enteroids in EL materials at 12 days post‐encapsulation as single cells. Two‐way ANOVA with Tukey multiple comparisons testing, * = p < 0.05, ** = p < 0.01, n = 3. f) Shear storage moduli of Stiff EL and Stiff Viscoelastic (VE) formulations. Student's t‐test, N = 3–5, n.s. = not significant. g) Step‐strain–stress relaxation curves comparing Stiff EL and Stiff VE formulations. h) Cross‐sectional area measurements of enteroids in stiff materials at 12 days post‐encapsulation as single cells. Two‐way ANOVA with Tukey multiple comparisons testing, * = p < 0.05, ** = p < 0.01, n = 3. All data shown are mean ± SD.