Cocoa Pod Husk (CPH) is the main by-product of cocoa pods (Theobroma cacao L.) with 67-76% of fruit weight. However, CPH has a negative impact if it is not utilized and disposed of directly in the environment. The main fiber content in CPH is in the form of lignin, cellulose, hemicellulose, and pectin. Cellulose content, especially α-cellulose has a high potential if it is further utilized, one of which is nanocellulose. This study aims to produce α-cellulose from cocoa husks with high purity. The first research activity carried out was the process of removing pectin and bleaching to be free from impurities such as pectin, lignin, and hemicellulose. Then the cellulose isolation process using Peracetic Acid (PAA) can shorten the α-cellulose isolation process. The variation of PAA concentration was 1:4 (mol/mol) without dilution; 1:4 (mole/mole) by dilution; and 1:1 (mole/mole). The results of this study were the highest α-cellulose content of 69.39% was obtained from a 1:4 mole ratio of PAA without dilution. However, the α-cellulose content obtained did not qualify the SNI 938-2017 standard, which was 94%. FTIR, XRD, and SEM characterization showed that α-cellulose was present in hydrolysed CPH.