The White House refused to discuss the library's location until Bush had secured a second term. In late 2005, six colleges and the city of Arlington, Texas, were invited to submit bids. Baylor University offered riverfront land on the Brazos River in Waco but lacked the visitor draw of a major metro area. Texas Tech and Midland College formed a 'West Texas Coalition' pitching Lubbock. The University of Texas System proposed a 'virtual library' split across multiple campuses -- an idea that generated a student newspaper editorial titled 'Don't waste funds on W's library.' The University of Dallas, a small Catholic school in Irving, had hundreds of acres of undeveloped land and ambitious plans including waterfalls and jogging trails. Then there was SMU, whose bid was 'mired in mystery,' especially regarding where it would find the land. The answer: buy it, one property at a time.

Not everyone at SMU was thrilled. In December 2006, members of the Perkins School of Theology wrote to the university president expressing concern that the library would serve as a 'conservative think tank that engages in legacy polishing.' A group of Methodists launched a petition calling it inappropriate to link Bush's presidency to a university bearing the Methodist name; The Guardian reported the petition gathered 12,500 signatures. Faculty complained about being left out of the decision. Despite the friction, SMU confirmed the agreement on February 22, 2008. Groundbreaking followed on November 16, 2010, timed with the release of Bush's memoir Decision Points. At the ceremony, former Vice President Dick Cheney quipped that the library 'may be the only shovel-ready project in America' -- a pointed reference to President Obama's stimulus package.

The center's museum includes a full-size replica of the Oval Office with the Resolute Desk, where visitors can pose for photographs. The main narrative arc is organized around the September 11, 2001, terrorist attacks, featuring artifacts from that day. An interactive exhibit called 'Decision Points,' named after the president's memoir, puts visitors in the position of weighing options during key moments of the Bush presidency, including Hurricane Katrina and the 2008 financial crisis. A collection of items from first ladies of the United States and a rotating temporary exhibit hall round out the displays. Bush's own paintings -- a post-presidential pursuit that surprised many -- are also exhibited. Outside, a 14-acre native garden dedicated to Laura Bush uses over 90 native Texan plant species and 900 native trees, supporting a lawn that achieves a biomass density 62 percent higher than a conventional landscape.

The George W. Bush Institute, housed within the center, operates as an 'action-oriented think tank' independent of SMU. Ambassador James K. Glassman, a former State Department official, served as its founding executive director from 2009 to 2013. The institute focuses on four causes: human freedom, global health, economic growth, and education reform. Laura Bush leads a women's initiative, and a military service initiative supports U.S. veterans. In early 2018, the institute received two $10 million endowments from Boeing and Highland Capital Management. At the November 2010 groundbreaking, Bush articulated his post-presidential philosophy: 'The decisions of governing are on another president's desk, and he deserves to make them without criticism from me. But staying out of current affairs and politics does not mean staying out of policy.'

The project ultimately raised over $500 million for construction and endowment, far exceeding its initial $300 million goal. The construction itself cost approximately $250 million, and the sustainable design features -- including a vegetative bioswale for stormwater management and irrigation systems that reduce potable water consumption by 75 percent -- earned it the highest possible LEED certification. In November 2022, the National Archives and Records Administration transferred museum operations to the George W. Bush Foundation, effective January 1, 2023. The transfer had been paused over concerns about whitewashing exhibits on controversial topics, a problem that had previously affected the Richard Nixon Presidential Library. Under the agreement, the foundation must obtain input from NARA and historians, clearly designate foundation and NARA spaces, and NARA retains ownership of all presidential artifacts on loan. The center is also designated as the eventual burial site of George W. Bush and Laura Bush.