On 16 October 2004, he made his La Liga debut with the main squad, coming on as a second-half substitute in a 1–1 away draw against Real Betis.

[7] On 24 July 2006, Arbeloa signed for Deportivo de La Coruña, with Real Madrid being entitled to 50% of any transfer occurring in the following three years.

On 17 May 2009, in a match against West Bromwich Albion, Arbeloa was involved in an on-field clash with teammate Jamie Carragher – the two had to be separated by Daniel Agger, Xabi Alonso, Emiliano Insúa and Pepe Reina.

[20] On 29 July 2009, it was announced that Real Madrid and Liverpool had reached an agreement on the transfer of Arbeloa, for a fee of £5 million and a five-year contract.

[24] Under new manager José Mourinho, he celebrated his tenth appearance in the Champions League with his first goal in the competition, netting from outside the penalty area in a 4–0 victory at AFC Ajax in the group stage.

[25] In the 2011–12 campaign, due to Ricardo Carvalho's lengthy injury, Sergio Ramos was relocated to centre-back and Arbeloa began appearing almost exclusively on the right side of the back four.

[39] On 1 February 2008, Arbeloa was called up to the Spanish national team for the first time, for a friendly with France in Málaga, but he was forced to pull out because of injury.

[40] He made his debut on 26 March against Italy,[41] and was picked for UEFA Euro 2008's final stages, appearing in the first-round match against Greece (2–1 win)[42] as the nation emerged victorious.

[44][45] Due to Carles Puyol's absence, however, he was now part of the starting XI alongside Ramos, Gerard Piqué and Jordi Alba, with Spain only conceding once in six fixtures and winning the tournament.