Artificial Intelligence (AI), particularly through the advent of large-scale generative AI (GenAI) models such as Large Language Models (LLMs), has become a transformative element in contemporary technology. While these models have unlocked new possibilities, they simultaneously present significant challenges, such as concerns over data privacy and the propensity to generate misleading or fabricated content. Current frameworks for Responsible AI (RAI) often fall short in providing the granular guidance necessary for tangible application, especially for \textit{Accountability}—a principle that is pivotal for ensuring transparent and auditable decision-making, bolstering public trust, and meeting increasing regulatory expectations. This study bridges the \textit{Accountability gap} by introducing a comprehensive metrics catalogue, formulated through a systematic multivocal literature review (MLR) that integrates findings from both academic and grey literature. Our catalogue delineates process metrics that underpin procedural integrity, resource metrics that provide necessary tools and frameworks, and product metrics that reflect the outputs of AI systems. This tripartite framework is designed to operationalize Accountability in AI, with a special emphasis on addressing the intricacies of GenAI. The proposed metrics catalogue provides a robust framework for instilling Accountability in AI systems. It offers practical, actionable guidance for organizations, thereby shaping responsible practices in the field.