Recent knowledge editing methods have primarily focused on modifying structured knowledge in large language models, heavily relying on the assumption that structured knowledge is stored as key-value pairs locally in MLP layers or specific neurons. However, this task setting overlooks the fact that a significant portion of real-world knowledge is stored in an unstructured format, characterized by long-form content, noise, and a complex yet comprehensive nature. The "knowledge locating" and "term-driven optimization" techniques conducted from the assumption used in previous methods (e.g., MEMIT) are ill-suited for unstructured knowledge. To address these challenges, we propose a novel unstructured knowledge editing method, namely UnKE, which extends previous assumptions in the layer dimension and token dimension. Firstly, in the layer dimension, we discard the "knowledge locating" step and treat first few layers as the key, which expand knowledge storage through layers to break the "knowledge stored locally" assumption. Next, we replace "term-driven optimization" with "cause-driven optimization" across all inputted tokens in the token dimension, directly optimizing the last layer of the key generator to perform editing to generate the required key vectors. By utilizing key-value pairs at the layer level, UnKE effectively represents and edits complex and comprehensive unstructured knowledge, leveraging the potential of both the MLP and attention layers. Results on newly proposed unstructure knowledge editing dataset (UnKEBench) and traditional structured datasets demonstrate that UnKE achieves remarkable performance, surpassing strong baselines.