This work presents an iterated improved reduced system (IIRS) procedure combined with sub-structuring scheme for large structures. Iterated IRS methods are usually more efficient than others because the dynamic condensation matrix is updated repeatedly until the desired convergent values are obtained. However, using these methods simply for large structures causes expensive computational cost and even makes analyses intractable because of the limited computer storage. Therefore, the application of sub-structuring scheme is necessary. Because the large structures are subdivided into several (or more) sub-domains, the construction of dynamic condensation matrix does not require much computation cost in every iteration. This makes the present method much more efficient to compute the eigenpairs both in lower and intermediate modes. In Part I, iterated IRS method combined with sub-structuring scheme for undamped structures is presented. The validation of the proposed method and the evaluation of computational efficiency are demonstrated through the numerical examples.