And the Netherlands look increasingly like credible pretenders for that newly vacated crown.
Just like France in 2002 and Italy in 2010, defending champion Spain is going home tail between its legs.
Chile delivered the mortal blow to an uninterrupted 6-year era of dominance for Spain, the European and world champions whose dazzling footballers ran out of puff in Brazil. They were made to look vulnerable last week in losing 5-1 to the Netherlands and then simply plain ordinary in a 2-0 loss to a physical and quick Chilean side.
The Netherlands, 3-2 winners against Australia on Wednesday, and Chile are now both sure to advance to the next knockout round having won their two first matches. They will now play each other Monday to determine which of them tops Group B and avoids a possible encounter with host Brazil in the first knockout game on June 28.
In Wednesday's evening game, Croatia ensured Cameroon won't go further, delivering a 4-0 thumping to the African side whose injured star, Samuel Eto'o, didn't come off the bench. This is shaping up as another tough World Cup for Africa. Only Ivory Coast has won so far - its opener, 2-1, against Japan. It plays Colombia in Group C on Thursday, with the other matches Uruguay vs. England in Group D and Japan vs. Greece in Group C.
With strikers Mario Mandzukic and Ivica Olic both scoring and midfielder Ivan Perisic getting a goal, too, Croatia presents a tough challenge for Mexico in their last Group A match next Monday. Mexico needs at least a draw to guarantee a place in the last 16. In the other Group A match, Brazil should have little difficulty against the feeble Cameroon side that was reduced to 10 men after 40 minutes against Croatia when Alex Song was shown red.
At the Maracana Stadium in Rio de Janeiro, fevered Chile fans yelling "It's over! It's over!" taunted Spanish supporters, some of them in tears, bitterly contemplating the end of an era for one of football's greatest ever teams. Its success - back-to-back European titles and the World Cup in 2010 - has provided succor in brutal economic times for Spaniards.
"The only happiness we've had in recent years has been football," said Beatriz Corral, who came to Rio from Madrid to cheer for Spain. "Now the crisis is complete. We don't have bread or the circus."
Demolishing Spain last week showed the Dutch can be spectacular. Toughing out a come-from-behind 3-2 victory against Australia showed them to also be resilient and cool under pressure - vital qualities for the knockout rounds.
Arjen Robben opened the scoring for the Netherlands before Tim Cahill brought the sides level a minute later with a stunning volley, one of the best strikes so far in the tournament that has seen 60 goals in 20 games.
Mile Jedinak then converted a 54th minute penalty and Robin van Persie equalized for the Netherlands with his third goal of the tournament. A goalkeeping blunder by Maty Ryan then handed substitute Memphis Depay his first international goal, the winner for the Netherlands.
With no points from its first two games, Spain will play only for pride when it meets Australia - also winless in its first two games - in their last match Group B match.
Then it will be "adios" and a return home to the inevitable post-mortem of how a team that played like clockwork in defending its European title two years ago could fall so far, so quickly.
In Brazil, the advancing age of key players, grievous mistakes from captain Iker Casillas and others, and coach Vicente del Bosque's failure to read the writing on the wall fatally threw the Spanish machine out of gear.
Spain's demise was also a reminder of how difficult it is to retain the World Cup and for coaches to keep teams fresh and motivated in the four-year gap between tournaments.
Only Italy - winners in 1934 and 1938 - and Brazil -champions in 1958 and 1962 - have won back-to-back World Cups.
Del Bosque came to Brazil with a goalkeeper, Casillas, who is no longer undisputed No. 1 at his club, Real Madrid, with a midfield playmaker, Xavi Hernandez, who at 34 is passed his peak, and with a new striker, Diego Costa, who has been a major disappointment, not finding the net once.
"We have no excuses," said del Bosque. "We were too slow, timid from the start today. It's a sad day for all of the players. Time to think about the future."