Materials with formula of A2B2O7 is a famous family with more than 300 compounds, and have abundant properties, like ferroelectric, multiferroic, and photocatalyst properties, etc. Generally, two structures dominate this family, which are pyrochlore and perovskite-like layered (PL) structure. Previously, the structure and properties design of these materials are usually complex, and solid solutions, which complicates the manufacture, as well as introducing complexity in the study of the microscopic origins of the properties. Here, we report that the pyrochlore-PL structure change happened in pure Eu2Ti2O7 under high pressure and temperature, and the formed PL structure will transfer back by heating. These results reveal that the PL structure formed in PL-pyrochlore solid solutions, is due to tuning of the high-pressure formed PL structure in pure pyrochlore compounds to ambient pressure. These results indicate the high pressure and high temperature can be used to manipulate the crystal structures from pyrochlore to PL structure, or vice versa. Furthermore, the PL Eu2Ti2O7 was confirmed as a lead free ferroelectric material for the first time.