Madrid suffer Villa and Ribery set-backs
"We have been in talks to buy Villa the past week but there has been no agreement," Valdano said in an interview with Spanish radio station Onda Cero.
"What appeared to be well on the way to happening looks now to be falling through," he added. "If there is no accord we still have two or three more alternatives."
Valdano, who was appointed to help oversee a massive spending project to help rebuild the team under new president Florentino Perez, said Bayern were playing hardball on the Ribery transfer.
"They don't want to sell him and that's why they quoted us an astronomical price," he said.
In Germany, Bayern reiterated their desire to hold on to Ribery with at least three other major European clubs retaining an interest in buying him.
Still under contract until 2011, the Frenchman has recently hinted he would like to play in Spain or England but his German employers are adamant he will stay on.
"We turned (a Real Madrid offer) down because we have no intention of selling Ribery," Bayern chairman Karl-Heinz Rummenigge told Bild newspaper, adding that the Spanish club did not specify an exact amount while other enquirers had.
"Other teams have confronted us with specific sums," Rummenigge said. "Chelsea have been in touch, as well as Manchester United and Barcelona."
Bayern said recently they would not consider any bids under 40 million euros for the 26-year-old France international.
"We did not buy Franck two years ago to cash in but to improve our team. Now we have to do everything for him to stay and I am determined to do that," Rummenigge said. "A player has to respect his contract, in this case until 2011."
Lyon striker Karim Benzema was another of Madrid's targets, but there was plenty of time before the end of the transfer period to negotiate a deal for the player, Valdano said.
It appeared the club's efforts to sign Liverpool and Spain midfielder Xabi Alonso would come to nothing as the English club did not want to sell him, he added.
Real were looking to buy four or five more players following the purchase of Kaka and the record bid for Cristiano Ronaldo, but further arrivals depended on the club selling players first, Valdano said.
"There are interesting offers for some players but many of them do not want to leave," he said.
The club had received the most offers for Dutch pair Arjen Robben and Wesley Sneijder, Valdano added, but suggested the amount of money on the table was not enough.