Anthropomorphic CT phantoms are essential training tools for interventional radiology. Given the high technical demands and stringent safety requirements in this field, realistic CT phantoms are vital simulation tools that support effective hands-on training, procedural planning, and risk mitigation. However, commercially available phantom geometries are limited in their scope. This study investigates the use of polyvinyl alcohol (PVA) to fabricate customizable training phantoms. PVA, a non-toxic material, can be processed into PVA cryogels (PVA-C) with tissue-like mechanical properties. We modified PVA-C (10 wt.% PVA) by incorporating various additives to adjust X-ray attenuation and achieve Hounsfield units (HUs) similar to different soft tissues. HU values were measured at X-ray tube voltages of 70, 120, and 150 kV. The inclusion of barium sulfate (e.g., U = 120 kV; 0.1–2 wt.%: 33.29 ± 5.45–323.72 ± 12.64 HU) and iohexol (e.g., U = 120 kV; 0.1–2 wt.%: 26.05 ± 4.74–161.99 ± 5.69 HU) significantly increased HU values. Iohexol produced more homogeneous HU distributions than barium sulfate and cellulose derivatives, with the latter having air gaps and inconsistencies. The tested formulations encompassed a wide range of soft tissue densities, with HU values varying significantly across the energy range (p < 0.001). While cellulose derivatives showed variable HU modulation, their primary role appears to be in modifying phantom texture and morphology rather than precise attenuation control. In conclusion, PVA-C demonstrates strong potential for use in interventional radiology training phantoms. Further studies may enhance phantom realism by replicating tissue textures, for example, through the incorporation of cellulose-based substances.