According to Spanish media, the accident occurred when the car carrying the two Jota brothers lost control, leading to a serious collision and a fire.
Although witnesses quickly called rescue forces, both victims could not survive.
Diogo Jota, 28, is a Liverpool player, while his younger brother, Andre Silva, 26, is playing for Penafiel club in Portugal.
In response to the great loss, the Portuguese Football Federation (FPF) issued an official statement: "The Portuguese Football Federation and the entire country's football scene are in dire pain at the departure of Diogo Jota and his younger brother Andre Silva. We have lost two champions.
Their passing is an irreparable loss. We are committed to preserving and honoring the heritage they left behind. The federation also suggested UEFA hold a minute of silence before the match between the Portuguese and Spanish women's teams at the upcoming EURO for women".
Many big clubs have also expressed their condolences. Portuguese club Sporting CP wrote: "The world of football is without good players. Sporting CP is extremely saddened. My deepest condolences to the entire family".
The former team of both brothers, FC Porto, also sent a message: "We are extremely shocked and saddened. I would like to send my deepest condolences to the family and friends of the two brothers".
The departure of Diogo Jota and Andre Silva is not only a loss for their family, but also a big gap for Portuguese football and the global football community. In the coming days, many commemorative activities are expected to be held to honor the two talented players.